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  • 1.
    Abrikossova, Natalia
    Linköping University, Department of Physics, Chemistry and Biology, Molecular Surface Physics and Nano Science. Linköping University, Faculty of Science & Engineering.
    Investigation of nanoparticle-cell interactions for development of next generation of biocompatible MRI contrast agents2018Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Progress in synthesis technologies and advances in fundamental understanding of materials with low dimensionality has led to the birth of a new scientific field, nanoscience, and to strong expectations of multiple applications of nanomaterials. The physical properties of small particles are unique, bridging the gap between atoms and molecules, on one side, and bulk materials on the other side. The work presented in this thesis investigates the potential of using magnetic nanoparticles as the next generation of contrast agents for biomedical imaging. The focus is on gadolinium-based nanoparticles and cellular activity including the uptake, morphology and production of reactive oxygen species.

    Gd ion complexes, like Gd chelates, are used today in the clinic, world-wide. However, there is a need for novel agents, with improved contrast capabilities and increased biocompatibility. One avenue in their design is based on crystalline nanoparticles. It allows to reduce the total number of Gd ions needed for an examination. This can be done by nanotechnology, which allows one to improve and fine tune the physico- chemical properties on the nanomaterial in use, and to increase the number of Gd atoms at a specific site that interact with protons and thereby locally increase the signal. In the present work, synthesis, purification and surface modification of crystalline Gd2O3-based nanoparticles have been performed. The nanoparticles are selected on the basis of their physical properties, that is they show enhanced magnetic properties and therefore may be of high potential interest for applications as contrast agents.

    The main synthesis method of Gd2O3 nanoparticles in this work was the modified “polyol” route, followed by purification of as-synthesized DEG-Gd2O3 nanoparticles suspensions. In most cases the purification step involved dialysis of the nanoparticle samples. In this thesis, organosilane were chosen as an exchange agent for further functionalization. Moreover, several paths have been explored for modification of the nanoparticles, including Tb3+ doping and capping with sorbitol.

    Biocompatibility of the newly designed nanoparticles is a prerequisite for their use in medical applications. Its evaluation is a complex process involving a wide range of biological phenomena. A promising path adopted in this work is to study of nanoparticle interactions with isolated blood cells. In this way one could screen nanomaterial prior to animal studies.

    The primary cell type considered in the thesis are polymorphonuclear neutrophils (PMN) which represent a type of the cells of human blood belonging to the granulocyte family of leukocytes. PMNs act as the first defense of the immune system against invading pathogens, which makes them valuable for studies of biocompatibility of newly synthesized nanoparticles. In addition, an immortalized murine alveolar macrophage cell line (MH-S), THP-1 cell line, and Ba/F3 murine bone marrow-derived cell line were considered to investigate the optimization of the cell uptake and to examine the potential of new intracellular contrast agent for magnetic resonance imaging.

    In paper I, the nanoparticles were investigated in a cellular system, as potential probes for visualization and targeting intended for bioimaging applications. The production of reactive oxygen species (ROS) by means of luminol-dependent chemiluminescence from human neutrophils was studied in presence of Gd2O3 nanoparticles. In paper II, a new design of functionalized ultra-small rare earth-based nanoparticles was reported. The synthesis was done using polyol method followed by PEGylation, and dialysis. Supersmall gadolinium oxide (DEG-Gd2O3) nanoparticles, in the range of 3-5 nm were obtained and carefully characterized. Neutrophil activation after exposure to this nanomaterial was studied by means of fluorescence microscopy. In paper III, cell labeling with Gd2O3 nanoparticles in hematopoietic cells was monitored by magnetic resonance imaging (MRI). In paper IV, ultra-small gadolinium oxide nanoparticles doped with terbium ions were synthesized as a potentially bifunctional material with both fluorescent and magnetic contrast agent properties. Paramagnetic behavior was studied. MRI contrast enhancement was received, and the luminescent/ fluorescent property of the particles was attributable to the Tb3+ ion located on the crystal lattice of the Gd2O3 host. Fluorescent labeling of living cells was obtained. In manuscript V, neutrophil granulocytes were investigated with rapid cell signaling communicative processes in time frame of minutes, and their response to cerium-oxide based nanoparticles were monitored using capacitive sensors based on Lab-on-a-chip technology. This showed the potential of label free method used to measure oxidative stress of neutrophil granulocytes. In manuscript VI, investigations of cell-(DEGGd2O3) nanoparticle interactions were carried out. Plain (DEG-Gd2O3) nanoparticles, (DEG-Gd2O3) nanoparticles in presence of sorbitol and (DEG-Gd2O3) nanoparticles capped with sorbitol were studied. Relaxation studies and measurements of the reactive oxygen species production by neutrophils were based on chemiluminescence. Cell morphology was evaluated as a parameter of the nanoparticle induced inflammatory response by means of the fluorescence microscopy.

    The thesis demonstrates high potential of novel Gd2O3-based nanoparticles for development of the next generation contrast agents, that is to find biocompatible compounds with high relaxivity that can be detected at lower doses, and in the future enable targeting to provide great local contrast.

    List of papers
    1. Effects of gadolinium oxide nanoparticles on the oxidative burst from human neutrophil granulocytes
    Open this publication in new window or tab >>Effects of gadolinium oxide nanoparticles on the oxidative burst from human neutrophil granulocytes
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    2012 (English)In: Nanotechnology, ISSN 0957-4484, E-ISSN 1361-6528, Vol. 23, no 27, p. 275101-Article in journal (Refereed) Published
    Abstract [en]

    We have previously shown that gadolinium oxide (Gd2O3) nanoparticles are promising candidates to be used as contrast agents in magnetic resonance (MR) imaging applications. In this study, these nanoparticles were investigated in a cellular system, as possible probes for visualization and targeting intended for bioimaging applications. We evaluated the impact of the presence of Gd2O3 nanoparticles on the production of reactive oxygen species (ROS) from human neutrophils, by means of luminol-dependent chemiluminescence. Three sets of Gd2O3 nanoparticles were studied, i.e. as synthesized, dialyzed and both PEG-functionalized and dialyzed Gd2O3 nanoparticles. In addition, neutrophil morphology was evaluated by fluorescent staining of the actin cytoskeleton and fluorescence microscopy. We show that surface modification of these nanoparticles with polyethylene glycol (PEG) is essential in order to increase their biocompatibility. We observed that the as synthesized nanoparticles markedly decreased the ROS production from neutrophils challenged with prey (opsonized yeast particles) compared to controls without nanoparticles. After functionalization and dialysis, more moderate inhibitory effects were observed at a corresponding concentration of gadolinium. At lower gadolinium concentration the response was similar to that of the control cells. We suggest that the diethylene glycol (DEG) present in the as synthesized nanoparticle preparation is responsible for the inhibitory effects on the neutrophil oxidative burst. Indeed, in the present study we also show that even a low concentration of DEG, 0.3%, severely inhibits neutrophil function. In summary, the low cellular response upon PEG-functionalized Gd2O3 nanoparticle exposure indicates that these nanoparticles are promising candidates for MR-imaging purposes.

    Place, publisher, year, edition, pages
    Institute of Physics, 2012
    National Category
    Engineering and Technology
    Identifiers
    urn:nbn:se:liu:diva-79667 (URN)10.1088/0957-4484/23/27/275101 (DOI)000305802000001 ()
    Available from: 2012-08-14 Created: 2012-08-13 Last updated: 2018-11-12
    2. Synthesis and Characterization of PEGylated Gd2O3 Nanoparticles for MRI Contrast Enhancement
    Open this publication in new window or tab >>Synthesis and Characterization of PEGylated Gd2O3 Nanoparticles for MRI Contrast Enhancement
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    2010 (English)In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 26, no 8, p. 5753-5762Article in journal (Refereed) Published
    Abstract [en]

    Recently, much attention has been given to the development of biofunctionalized nanoparticles with magnetic properties for novel biomedical imaging. Guided, smart, targeting nanoparticulate magnetic resonance imaging (MRI) contrast agents inducing high MRI signal will be valuable tools for future tissue specific imaging and investigation of molecular and cellular events. In this study, we report a new design of functionalized ultrasmall rare earth based nanoparticles to be used as a positive contrast agent in MRI. The relaxivity is compared to commercially available Gd based chelates. The synthesis, PEGylation, and dialysis of small (3−5 nm) gadolinium oxide (DEG-Gd2O3) nanoparticles are presented. The chemical and physical properties of the nanomaterial were investigated with Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, transmission electron microscopy, and dynamic light scattering. Neutrophil activation after exposure to this nanomaterial was studied by means of fluorescence microscopy. The proton relaxation times as a function of dialysis time and functionalization were measured at 1.5 T. A capping procedure introducing stabilizing properties was designed and verified, and the dialysis effects were evaluated. A higher proton relaxivity was obtained for as-synthesized diethylene glycol (DEG)-Gd2O3 nanoparticles compared to commercial Gd-DTPA. A slight decrease of the relaxivity for as-synthesized DEG-Gd2O3 nanoparticles as a function of dialysis time was observed. The results for functionalized nanoparticles showed a considerable relaxivity increase for particles dialyzed extensively with r1 and r2 values approximately 4 times the corresponding values for Gd-DTPA. The microscopy study showed that PEGylated nanoparticles do not activate neutrophils in contrast to uncapped Gd2O3. Finally, the nanoparticles are equipped with Rhodamine to show that our PEGylated nanoparticles are available for further coupling chemistry, and thus prepared for targeting purposes. The long term goal is to design a powerful, directed contrast agent for MRI examinations with specific targeting possibilities and with properties inducing local contrast, that is, an extremely high MR signal at the cellular and molecular level.

    Place, publisher, year, edition, pages
    American Chemical Society (ACS), 2010
    National Category
    Natural Sciences
    Identifiers
    urn:nbn:se:liu:diva-54946 (URN)10.1021/la903566y (DOI)000276562300061 ()
    Available from: 2010-04-23 Created: 2010-04-23 Last updated: 2018-10-29Bibliographically approved
    3. Gd2O3 nanoparticles in hematopoietic cells for MRI contrast enhancement
    Open this publication in new window or tab >>Gd2O3 nanoparticles in hematopoietic cells for MRI contrast enhancement
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    2011 (English)In: International journal of nano medicine, ISSN 1178-2013, Vol. 6, p. 3233-3240Article in journal (Refereed) Published
    Abstract [en]

    As the utility of magnetic resonance imaging (MRI) broadens, the importance of having specific and efficient contrast agents increases and in recent time there has been a huge development in the fields of molecular imaging and intracellular markers. Previous studies have shown that gadolinium oxide (Gd2O3) nanoparticles generate higher relaxivity than currently available Gd chelates: In addition, the Gd2O3 nanoparticles have promising properties for MRI cell tracking. The aim of the present work was to study cell labeling with Gd2O3 nanoparticles in hematopoietic cells and to improve techniques for monitoring hematopoietic stem cell migration by MRI. Particle uptake was studied in two cell lines: the hematopoietic progenitor cell line Ba/F3 and the monocytic cell line THP-1. Cells were incubated with Gd2O3 nanoparticles and it was investigated whether the transfection agent protamine sulfate increased the particle uptake. Treated cells were examined by electron microscopy and MRI, and analyzed for particle content by inductively coupled plasma sector field mass spectrometry. Results showed that particles were intracellular, however, sparsely in Ba/F3. The relaxation times were shortened with increasing particle concentration. Relaxivities, r1 and r2 at 1.5 T and 21°C, for Gd2O3 nanoparticles in different cell samples were 3.6–5.3 s-1 mM-1 and 9.6–17.2 s-1 mM-1, respectively. Protamine sulfate treatment increased the uptake in both Ba/F3 cells and THP-1 cells. However, the increased uptake did not increase the relaxation rate for THP-1 as for Ba/F3, probably due to aggregation and/or saturation effects. Viability of treated cells was not significantly decreased and thus, it was concluded that the use of Gd2O3 nanoparticles is suitable for this type of cell labeling by means of detecting and monitoring hematopoietic cells. In conclusion, Gd2O3 nanoparticles are a promising material to achieve positive intracellular MRI contrast; however, further particle development needs to be performed.

    Place, publisher, year, edition, pages
    Manchester, UK: Dove Medical Press Ltd, 2011
    Keywords
    gadolinium oxide, magnetic resonance imaging, contrast agent, cell labeling, Ba/F3 cells, THP-1 cells
    National Category
    Medical and Health Sciences
    Identifiers
    urn:nbn:se:liu:diva-72275 (URN)10.2147/IJN.S23940 (DOI)000298164300001 ()
    Note

    funding agencies|Swedish Research Council| 621-2007-3810 621-2009-5148 521-2009-3423 |VINNOVA| 2009-00194 |Center in Nanoscience and Technology at LiTH (CeNano)||

    Available from: 2011-11-24 Created: 2011-11-24 Last updated: 2018-10-29
    4. Synthesis and Characterization of Tb3+-Doped Gd2O3 Nanocrystals: A Bifunctional Material with Combined Fluorescent Labeling and MRI Contrast Agent Properties
    Open this publication in new window or tab >>Synthesis and Characterization of Tb3+-Doped Gd2O3 Nanocrystals: A Bifunctional Material with Combined Fluorescent Labeling and MRI Contrast Agent Properties
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    2009 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 113, no 17, p. 6913-6920Article in journal (Refereed) Published
    Abstract [en]

    Ultrasmall gadolinium oxide nanoparticles doped with terbium ions were synthesized by the polyol route and characterized as a potentially bifunctional material with both fluorescent and magnetic contrast agent properties. The structural, optical, and magnetic properties of the organic-acid-capped and PEGylated Gd2O3:Tb3+ nanocrystals were studied by HR-TEM, XPS, EDX, IR, PL, and SQUID. The luminescent/fluorescent property of the particles is attributable to the Tb3+ ion located on the crystal lattice of the Gd2O3 host. The paramagnetic behavior of the particles is discussed. Pilot studies investigating the capability of the nanoparticles for fluorescent labeling of living cells and as a MRI contrast agent were also performed. Cells of two cell lines (THP-1 cells and fibroblasts) were incubated with the particles, and intracellular particle distribution was visualized by confocal microscopy. The MRI relaxivity of the PEGylated nanoparticles in water at low Gd concentration was assessed showing a higher T-1 relaxation rate compared to conventional Gd-DTPA chelates and comparable to that of undoped Gd2O3 nanoparticles.

    National Category
    Natural Sciences
    Identifiers
    urn:nbn:se:liu:diva-12944 (URN)10.1021/jp808708m (DOI)000265529700009 ()
    Note

    On the day of the defence date the status of this article was Submitted

    Available from: 2008-02-21 Created: 2008-02-21 Last updated: 2018-10-29Bibliographically approved
  • 2.
    Ahmadkhaniha, D.
    et al.
    Jonkoping Univ, Sweden.
    Eriksson, Fredrik
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Leisner, P.
    Jonkoping Univ, Sweden; RISE Res Inst Sweden, Sweden.
    Zanella, C.
    Jonkoping Univ, Sweden.
    Effect of SiC particle size and heat-treatment on microhardness and corrosion resistance of NiP electrodeposited coatings2018In: Journal of Alloys and Compounds, ISSN 0925-8388, E-ISSN 1873-4669, Vol. 769, p. 1080-1087Article in journal (Refereed)
    Abstract [en]

    Electrodeposition of NiP composite coatings with nano and sub-micron sized SiC has been carried out to investigate the possibility of replacing hard chromium coatings. The composition and structure of the coatings were evaluated by energy dispersive X-ray spectroscopy (EDS) and X-ray diffraction (XRD) analysis, respectively. Microhardness was measured by Vickers indentation and polarization measurements were carried out to study the corrosion behavior of the coatings. The results showed that submicron particles can be codeposited with a higher content as compared to nano sized ones. However, even if a smaller amount of the nano-sized SiC particles are incorporated in the coating, the contribution to an increasing microhardness was comparable with the submicron sized particles, which can be related to the higher density of codeposited particles. SiC particles did not change the anodic polarization behavior of NiP coatings in a 3.5% NaCl solution. Finally, the effect of heat-treatment on the coatings properties at 400 degrees C for 1 h was studied to investigate the contribution of particles and heat-treatment on hardness and corrosion properties. It was found that the heat-treatment doubled the microhardness and changed the anodic polarization behavior of the coatings from passive to active with respect to the asplated conditions. (C) 2018 Elsevier B.V. All rights reserved.

  • 3.
    Ahsan, Aisha
    et al.
    Univ Basel, Switzerland.
    Mousavi, S. Fatemeh
    Univ Basel, Switzerland.
    Nijs, Thomas
    Univ Basel, Switzerland.
    Nowakowska, Sylwia
    Univ Basel, Switzerland.
    Popova, Olha
    Univ Basel, Switzerland.
    Wackerlin, Aneliia
    Univ Basel, Switzerland.
    Björk, Jonas
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Gade, Lutz H.
    Heidelberg Univ, Germany.
    Jung, Thomas A.
    Univ Basel, Switzerland; Paul Scherrer Inst, Switzerland.
    Watching nanostructure growth: kinetically controlled diffusion and condensation of Xe in a surface metal organic network2019In: Nanoscale, ISSN 2040-3364, E-ISSN 2040-3372, Vol. 11, no 11, p. 4895-4903Article in journal (Refereed)
    Abstract [en]

    Diffusion, nucleation and growth provide the fundamental access to control nanostructure growth. In this study, the temperature activated diffusion of Xe at and between different compartments of an on-surface metal organic coordination network on Cu(111) has been visualized in real space. Xe atoms adsorbed at lower energy sites become mobile with increased temperature and gradually populate energetically more favourable binding sites or remain in a delocalized fluid form confined to diffusion along a topological subset of the on-surface network. These diffusion pathways can be studied individually under kinetic control via the chosen thermal energy kT of the sample and are determined by the network and sample architecture. The spatial distribution of Xe in its different modes of mobility and the time scales of the motion is revealed by Scanning Tunneling Microscopy (STM) at variable temperatures up to 40 K and subsequent cooling to 4 K. The system provides insight into the diffusion of a van der Waals gas on a complex structured surface and its nucleation and coarsening/growth into larger condensates at elevated temperature under thermodynamic conditions.

  • 4.
    Aijaz, Asim
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Plasma and Coating Physics. Linköping University, The Institute of Technology. Uppsala University, Sweden.
    Louring, Sascha
    Aarhus University, Denmark; Danish Technology Institute, Denmark.
    Lundin, Daniel
    University of Paris Saclay, France.
    Kubart, Tomas
    Uppsala University, Sweden.
    Jensen, Jens
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Sarakinos, Kostas
    Linköping University, Department of Physics, Chemistry and Biology, Nanoscale engineering. Linköping University, Faculty of Science & Engineering.
    Helmersson, Ulf
    Linköping University, Department of Physics, Chemistry and Biology, Plasma and Coating Physics. Linköping University, Faculty of Science & Engineering.
    Synthesis of hydrogenated diamondlike carbon thin films using neon-acetylene based high power impulse magnetron sputtering discharges2016In: Journal of Vacuum Science & Technology. A. Vacuum, Surfaces, and Films, ISSN 0734-2101, E-ISSN 1520-8559, Vol. 34, no 6, article id 061504Article in journal (Refereed)
    Abstract [en]

    Hydrogenated diamondlike carbon (DLC:H) thin films exhibit many interesting properties that can be tailored by controlling the composition and energy of the vapor fluxes used for their synthesis. This control can be facilitated by high electron density and/or high electron temperature plasmas that allow one to effectively tune the gas and surface chemistry during film growth, as well as the degree of ionization of the film forming species. The authors have recently demonstrated by adding Ne in an Ar-C high power impulse magnetron sputtering (HiPIMS) discharge that electron temperatures can be effectively increased to substantially ionize C species [Aijaz et al., Diamond Relat. Mater. 23, 1 (2012)]. The authors also developed an Ar-C2H2 HiPIMS process in which the high electron densities provided by the HiPIMS operation mode enhance gas phase dissociation reactions enabling control of the plasma and growth chemistry [Aijaz et al., Diamond Relat. Mater. 44, 117 (2014)]. Seeking to further enhance electron temperature and thereby promote electron impact induced interactions, control plasma chemical reaction pathways, and tune the resulting film properties, in this work, the authors synthesize DLC: H thin films by admixing Ne in a HiPIMS based Ar/C2H2 discharge. The authors investigate the plasma properties and discharge characteristics by measuring electron energy distributions as well as by studying discharge current characteristics showing an electron temperature enhancement in C2H2 based discharges and the role of ionic contribution to the film growth. These discharge conditions allow for the growth of thick (amp;gt;1 mu m) DLC: H thin films exhibiting low compressive stresses (similar to 0.5 GPa), high hardness (similar to 25 GPa), low H content (similar to 11%), and density in the order of 2.2 g/cm(3). The authors also show that film densification and change of mechanical properties are related to H removal by ion bombardment rather than subplantation. (C) 2016 American Vacuum Society.

  • 5.
    Ail, Ujwala
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Ullah Khan, Zia
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Granberg, Hjalmar
    Innventia AB, Sweden.
    Berthold, Fredrik
    Innventia AB, Sweden.
    Parasuraman, Rajasekar
    Mat Research Centre, India.
    Urnarji, Arun M.
    Mat Research Centre, India.
    Slettengren, Kerstin
    Innventia AB, Sweden.
    Pettersson, Henrik
    Innventia AB, Sweden.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Room temperature synthesis of transition metal silicide-conducting polymer micro-composites for thermoelectric applications2017In: Synthetic metals, ISSN 0379-6779, E-ISSN 1879-3290, Vol. 225, p. 55-63Article in journal (Refereed)
    Abstract [en]

    Organic polymer thermoelectrics (TE) as well as transition metal (TM) silicides are two thermoelectric class of materials of interest because they are composed of atomic elements of high abundatice; which is a prerequisite for mass implementation of thermoelectric (TE) solutions for solar and waste heat recovery. But both materials have drawbacks when it comes to finding low-cost manufacturing. The metal silicide needs high temperature (amp;gt;1000 degrees C) for creating TE legs in a device from solid powder, but it is easy to achieve long TE legs in this case. On the contrary, organic TEs are synthesized at low temperature from solution. However, it is difficult to form long legs or thick films because of their low solubility. In this work, we propose a novel method for the room temperature synthesis of TE composite containing the microparticles of chromium disilicide; CrSi2 (inorganic filler) in an organic matrix of nanofibrillated cellulose-poly(3,4-ethyelenedioxythiophene)-polystyrene sulfonate (NFC-PEDOT:PSS). With this method, it is easy to create long TE legs in a room temperature process. The originality of the approach is the use of conducting polymer aerogel microparticles mixed with CrSi2 microparticles to obtain a composite solid at room temperature under pressure. We foresee that the method can be scaled up to fabricate and pattern TE modules. The composite has an electrical conductivity (sigma) of 5.4 +/- 0.5 S/cm and the Seebeck coefficient (a) of 88 +/- 9 mu V/K, power factor (alpha(2)sigma) of 4 +/- 1 mu Wm(-1) K-2 at room temperature. At a temperature difference of 32 degrees C, the output power/unit area drawn across the load, with the resistance same as the internal resistance of the device is 0.6 +/- 0.1 mu W/cm(2). (C) 2017 Elsevier B.V. All rights reserved.

  • 6.
    Ajjan, Fátima
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Javad Jafari, Mohammad
    Linköping University, Department of Physics, Chemistry and Biology, Molecular Physics. Linköping University, Faculty of Science & Engineering.
    Rebis, T.
    Poznan University of Tech, Poland.
    Ederth, Thomas
    Linköping University, Department of Physics, Chemistry and Biology, Molecular Physics. Linköping University, Faculty of Science & Engineering.
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Spectroelectrochemical investigation of redox states in a polypyrrole/lignin composite electrode material2015In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 3, no 24, p. 12927-12937Article in journal (Refereed)
    Abstract [en]

    We report spectroelectrochemical studies to investigate the charge storage mechanism of composite polypyrrole/lignin electrodes. Renewable bioorganic electrode materials were produced by electropolymerization of pyrrole in the presence of a water-soluble lignin derivative acting as a dopant. The resulting composite exhibited enhanced charge storage abilities due to a lignin-based faradaic process, which was expressed after repeated electrochemical redox of the material. The in situ FTIR spectroelectrochemistry results show the formation of quinone groups, and reversible oxidation-reduction of these groups during charge-discharge experiments in the electrode materials. The most significant IR bands include carbonyl absorption near 1705 cm(-1), which is attributed to the creation of quinone moieties during oxidation, and absorption at 1045 cm(-1) which is due to hydroquinone moieties.

  • 7.
    Ajjan Godoy, Fátima Nadia
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Biohybrid Polymer Electrodes for Renewable Energy Storage2017Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Daily and seasonally fluctuating energy supply and demand requires adequate energy storage solutions. In recent years electrochemical supercapacitors have attracted considerable attention due to their ability to both store and deliver electrical energy efficiently. Our efforts are focused on developing and optimizing sustainable organic electrode materials for supercapacitors based on renewable bioorganic materials, offering a cheap, environmentally friendly and scalable alternative to store energy. In particular, we are using the second most abundant biopolymer in nature, lignin (Lig), which is an insulating material. However, when used in combination with electroactive and conducting polymers such as polypyrrole (PPy) and poly(3,4-ethylenedioxythiophene) (PEDOT), the biohybrid electrodes PPy/Lig and PEDOT/Lig display significantly enhanced energy storage performance as compared to the pristine conducting polymers without the lignin. Redox cyclic voltammetry and galvanostatic charge/discharge measurements indicate that the enhanced performance is due to the additional pseudocapacitance generated by the quinone moieties in lignin. Moreover, a conjugated redoxpolymer poly(aminoanthraquinone) PAAQ, with intrinsic quinone functions and excellentstability, has been combined with lignin and PEDOT resulting in a trihybrid bioelectrode. PEDOT compensates the low conductivity of PAAQ and provides electrical pathways to the quinone groups. The electrochemically generated quinones undergo a two electron, two protonredox process within the biohybrid electrodes as revealed by FTIR spectroelectrochemistry.These remarkable features reveal the exciting potential of a full organic energy storage device with long cycle life. Therefore, supercapacitor devices were designed in symmetric or asymmetric two electrode configuration. The best electrochemical performance was achieved by the asymmetric supercapacitor based on PEDOT+Lignin/PAAQ as the positive electrode and PEDOT/PAAQ as the negative electrode. This device exhibits superior electrochemical performance and outstanding stability after 10000 charge/discharge cycles due to the synergistic effect of the two electrodes. Finally, we have characterized the response of this supercapacitor device when charged with the intermittent power supply from an organic photovoltaic module. We have designed charging/discharging conditions such that reserve power was available in the storage device at all times. This work has resulted in an inexpensive fully organic system witht he dual function of energy conversion and storage.

    List of papers
    1. Biopolymer hybrid electrodes for scalable electricity storage
    Open this publication in new window or tab >>Biopolymer hybrid electrodes for scalable electricity storage
    2016 (English)In: Materials Horizons, ISSN 2051-6347, E-ISSN 2051-6355, Vol. 3, no 3, p. 174-185Article, review/survey (Refereed) Published
    Abstract [en]

    Powering the future, while maintaining a cleaner environment and a strong socioeconomic growth, is going to be one of the biggest challenges faced by mankind in the 21st century. The first step in overcoming the challenge for a sustainable future is to use energy more efficiently so that the demand for fossil fuels can be reduced drastically. The second step is a transition from the use of fossil fuels to renewable energy sources. In this sense, organic electrode materials are becoming increasingly attractive compared to inorganic electrode materials which have reached a plateau regarding performance and have severe drawbacks in terms of cost, safety and environmental friendliness. Using organic composites based on conducting polymers, such as polypyrrole, and abundant, cheap and naturally occurring biopolymers rich in quinones, such as lignin, has recently emerged as an interesting alternative. These materials, which exhibit electronic and ionic conductivity, provide challenging opportunities in the development of new charge storage materials. This review presents an overview of recent developments in organic biopolymer composite electrodes as renewable electroactive materials towards sustainable, cheap and scalable energy storage devices.

    Place, publisher, year, edition, pages
    ROYAL SOC CHEMISTRY, 2016
    National Category
    Other Environmental Engineering
    Identifiers
    urn:nbn:se:liu:diva-128741 (URN)10.1039/c5mh00261c (DOI)000375296600002 ()
    Note

    Funding Agencies|Knut and Alice Wallenberg Foundation; Wallenberg Scholar grant

    Available from: 2016-05-31 Created: 2016-05-30 Last updated: 2017-11-30
    2. Spectroelectrochemical investigation of redox states in a polypyrrole/lignin composite electrode material
    Open this publication in new window or tab >>Spectroelectrochemical investigation of redox states in a polypyrrole/lignin composite electrode material
    Show others...
    2015 (English)In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 3, no 24, p. 12927-12937Article in journal (Refereed) Published
    Abstract [en]

    We report spectroelectrochemical studies to investigate the charge storage mechanism of composite polypyrrole/lignin electrodes. Renewable bioorganic electrode materials were produced by electropolymerization of pyrrole in the presence of a water-soluble lignin derivative acting as a dopant. The resulting composite exhibited enhanced charge storage abilities due to a lignin-based faradaic process, which was expressed after repeated electrochemical redox of the material. The in situ FTIR spectroelectrochemistry results show the formation of quinone groups, and reversible oxidation-reduction of these groups during charge-discharge experiments in the electrode materials. The most significant IR bands include carbonyl absorption near 1705 cm(-1), which is attributed to the creation of quinone moieties during oxidation, and absorption at 1045 cm(-1) which is due to hydroquinone moieties.

    Place, publisher, year, edition, pages
    ROYAL SOC CHEMISTRY, 2015
    National Category
    Materials Chemistry
    Identifiers
    urn:nbn:se:liu:diva-120069 (URN)10.1039/c5ta00788g (DOI)000356022800044 ()
    Note

    Funding Agencies|Knut and Alice Wallenberg foundation; Marie Curie network Renaissance; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [2009-00971]

    Available from: 2015-07-06 Created: 2015-07-06 Last updated: 2017-12-04
    3. High performance PEDOT/lignin biopolymer composites for electrochemical supercapacitors
    Open this publication in new window or tab >>High performance PEDOT/lignin biopolymer composites for electrochemical supercapacitors
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    2016 (English)In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 4, no 5, p. 1838-1847Article in journal (Refereed) Published
    Abstract [en]

    Developing sustainable organic electrode materials for energy storage applications is an urgent task. We present a promising candidate based on the use of lignin, the second most abundant biopolymer in nature. This polymer is combined with a conducting polymer, where lignin as a polyanion can behave both as a dopant and surfactant. The synthesis of PEDOT/Lig biocomposites by both oxidative chemical and electrochemical polymerization of EDOT in the presence of lignin sulfonate is presented. The characterization of PEDOT/Lig was performed by UV-Vis-NIR spectroscopy, FTIR infrared spectroscopy, thermogravimetric analysis, scanning electron microscopy, cyclic voltammetry and galvanostatic charge-discharge. PEDOT doped with lignin doubles the specific capacitance (170.4 F g(-1)) compared to reference PEDOT electrodes (80.4 F g(-1)). The enhanced energy storage performance is a consequence of the additional pseudocapacitance generated by the quinone moieties in lignin, which give rise to faradaic reactions. Furthermore PEDOT/Lig is a highly stable biocomposite, retaining about 83% of its electroactivity after 1000 charge/discharge cycles. These results illustrate that the redox doping strategy is a facile and straightforward approach to improve the electroactive performance of PEDOT.

    Place, publisher, year, edition, pages
    ROYAL SOC CHEMISTRY, 2016
    National Category
    Biological Sciences
    Identifiers
    urn:nbn:se:liu:diva-125323 (URN)10.1039/c5ta10096h (DOI)000368839200035 ()
    Note

    Funding Agencies|Power Papers project from the Knut and Alice Wallenberg foundation; Wallenberg Scholar grant from the Knut and Alice Wallenberg foundation; Marie Curie network Renaissance (NA); European Research Council by Starting Grant Innovative Polymers for Energy Storage (iPes) [306250]; Basque Government

    Available from: 2016-02-23 Created: 2016-02-19 Last updated: 2017-11-30
  • 8.
    Ali, Gulzar
    et al.
    University of Sindh, Pakistan.
    Tahira, Aneela
    Luleå University of Technology, Sweden.
    Begum Mallah, Arfana
    University of Sindh, Pakistan.
    Ahmed Mallah, Sarfraz
    University of Sindh, Pakistan.
    Ibupoto, Akila
    Shah Abdul Latif University, Pakistan.
    Ahmed Khand, Aftab
    Tsinghua University, Peoples R China.
    Baradi, Waryani
    University of Sindh, Pakistan.
    Willander, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Yu, Cong
    Chinese Academic Science, Peoples R China.
    Hussain Ibupoto, Zafar
    University of Sindh, Pakistan; Chinese Academic Science, Peoples R China.
    Functional CuO Microstructures for Glucose Sensing2018In: Journal of Electronic Materials, ISSN 0361-5235, E-ISSN 1543-186X, Vol. 47, no 2, p. 1519-1525Article in journal (Refereed)
    Abstract [en]

    CuO microstructures are produced in the presence of water-soluble amino acids by hydrothermal method. The used amino acids include isoleucine, alpha alanine, and arginine as a soft template and are used for tuning the morphology of CuO nanostructures. The crystalline and morphological investigations were carried out by x-ray diffraction (XRD) and scanning electron microscopy techniques. The XRD study has shown that CuO material obtained in the presence of different amino acids is of high purity and all have the same crystal phase. The CuO microstructures prepared in the presence of arginine were used for the development of sensitive and selective glucose biosensor. The linear range for the glucose detection are from 0.001 mM to 30 mM and limit of detection was found to be 0.0005 mM. The sensitivity was estimated around 77 mV/decade. The developed biosensor is highly selective, sensitive, stable and reproducible. The glucose biosensor was used for the determination of real human blood samples and the obtained results are satisfactory. The CuO material is functional therefore can be capitalized in wide range of applications such as lithium ion batteries, all oxide solar cells and supercapacitors.

  • 9.
    Ali, Sharafat
    et al.
    Linnaeus University, Sweden; Corning Inc, NY 14831 USA.
    Paul, Biplab
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Magnusson, Roger
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Broitman, Esteban
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering.
    Jonson, Bo
    Linnaeus University, Sweden.
    Eklund, Per
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Birch, Jens
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Synthesis and characterization of the mechanical and optical properties of Ca-Si-O-N thin films deposited by RF magnetron sputtering2017In: Surface & Coatings Technology, ISSN 0257-8972, E-ISSN 1879-3347, Vol. 315, p. 88-94Article in journal (Refereed)
    Abstract [en]

    Ca-Si-O-N thin films were deposited on commercial soda-lime silicate float glass, silica wafers and sapphire substrates by RF magnetron co-sputtering from Ca and Si targets in an Ar/N-2/O-2 gas mixture. Chemical composition, surface morphology, hardness, reduced elastic modulus and optical properties of the films were investigated using X-ray photoelectron spectroscopy, scanning electron microscopy, nanoindentation, and spectroscopic ellipsometry. It was found that the composition of the films can be controlled by the Ca target power, predominantly, and by the reactive gas flow. Thin films in the Ca-Si-O-N system are composed of N and Ca contents up to 31 eq. % and 60 eq. %, respectively. The films thickness ranges from 600 to 3000 nm and increases with increasing Ca target power. The films surface roughness varied between 2 and 12 nm, and approximately decreases with increasing power of Ca target. The hardness (4-12 GPa) and reduced elastic modulus (65-145 GPa) of the films increase and decrease with the N and Ca contents respectively. The refractive index (1.56-1.82) is primarily dictated by the N content. The properties are compared with findings for bulk glasses in the Ca-Si-(Al)-O-N systems, and it is concluded that Ca-Si-O-N thin films have higher values of hardness, elastic modulus and refractive index than bulk glasses of similar composition. (C) 2017 Elsevier B.V. All rights reserved.

  • 10.
    Alnoor, Hatim
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Toward the Optimization of Low-temperature Solution-based Synthesis of ZnO Nanostructures for Device Applications2017Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    One-dimensional (1D) nanostructures (NSs) of Zinc Oxide (ZnO) such as nanorods (NRs) have recently attracted considerable research attention due to their potential for the development of optoelectronic devices such as ultraviolet (UV) photodetectors and light-emitting diodes (LEDs). The potential of ZnO NRs in all these applications, however, would require synthesis of high crystal quality ZnO NRs with precise control over the optical and electronic properties. It is known that the optical and electronic properties of ZnO NRs are mostly influenced by the presence of native (intrinsic) and impurities (extrinsic) defects. Therefore, understanding the nature of these intrinsic and extrinsic defects and their spatial distribution is critical for optimizing the optical and electronic properties of ZnO NRs. However, identifying the origin of such defects is a complicated matter, especially for NSs, where the information on anisotropy is usually lost due to the lack of coherent orientation.

    Thus, the aim of this thesis is towards the optimization of the lowtemperature solution-based synthesis of ZnO NRs for device applications. In this connection, we first started with investigating the effect of the precursor solution stirring durations on the deep level defects concentration and their spatial distribution along the ZnO NRs. Then, by choosing the optimal stirring time, we studied the influence of ZnO seeding layer precursor’s types, and its molar ratios on the density of interface defects. The findings of these investigations were used to demonstrate ZnO NRs-based heterojunction LEDs. The ability to tune the point defects along the NRs enabled us further to incorporate cobalt (Co) ions into the ZnO NRs crystal lattice, where these ions could occupy the vacancies or interstitial defects through substitutional or interstitial doping. Following this, high crystal quality vertically welloriented ZnO NRs have been demonstrated by incorporating a small amount of Co into the ZnO crystal lattice. Finally, the influence of Co ions incorporation on the reduction of core-defects (CDs) in ZnO NRs was systematically examined using electron paramagnetic resonance (EPR).

    List of papers
    1. Effect of precursor solutions stirring on deep level defects concentration and spatial distribution in low temperature aqueous chemical synthesis of zinc oxide nanorods
    Open this publication in new window or tab >>Effect of precursor solutions stirring on deep level defects concentration and spatial distribution in low temperature aqueous chemical synthesis of zinc oxide nanorods
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    2015 (English)In: AIP Advances, ISSN 2158-3226, E-ISSN 2158-3226, Vol. 5, no 8, article id 087180Article in journal (Refereed) Published
    Abstract [en]

    Hexagonal c-axis oriented zinc oxide (ZnO) nanorods (NRs) with 120-300 nm diameters are synthesized via the low temperature aqueous chemical route at 80 degrees C on silver-coated glass substrates. The influence of varying the precursor solutions stirring durations on the concentration and spatial distributions of deep level defects in ZnO NRs is investigated. Room temperature micro-photoluminesnce (mu-PL) spectra were collected for all samples. Cathodoluminescence (CL) spectra of the as-synthesized NRs reveal a significant change in the intensity ratio of the near band edge emission (NBE) to the deep-level emission (DLE) peaks with increasing stirring durations. This is attributed to the variation in the concentration of the oxygen-deficiency with increasing stirring durations as suggested from the X-ray photoelectron spectroscopy analysis. Spatially resolved CL spectra taken along individual NRs revealed that stirring the precursor solutions for relatively short duration (1-3 h), which likely induced high super saturation under thermodynamic equilibrium during the synthesis process, is observed to favor the formation of point defects moving towards the tip of the NRs. In contrary, stirring for longer duration (5-15 h) will induce low super saturation favoring the formation of point defects located at the bottom of the NRs. These findings demonstrate that it is possible to control the concentration and spatial distribution of deep level defects in ZnO NRs by varying the stirring durations of the precursor solutions.

    Place, publisher, year, edition, pages
    AMER INST PHYSICS, 2015
    National Category
    Condensed Matter Physics
    Identifiers
    urn:nbn:se:liu:diva-122070 (URN)10.1063/1.4929981 (DOI)000360655900089 ()
    Note

    Funding Agencies|Avdanced Functional Materials (AFM) SFO project at Linkoping Univeristy, Sweden

    Available from: 2015-12-18 Created: 2015-10-19 Last updated: 2017-12-01
    2. Influence of ZnO seed layer precursor molar ratio on the density of interface defects in low temperature aqueous chemically synthesized ZnO nanorods/GaN light-emitting diodes
    Open this publication in new window or tab >>Influence of ZnO seed layer precursor molar ratio on the density of interface defects in low temperature aqueous chemically synthesized ZnO nanorods/GaN light-emitting diodes
    Show others...
    2016 (English)In: Journal of Applied Physics, ISSN 0021-8979, E-ISSN 1089-7550, Vol. 119, no 16, p. 165702-Article in journal (Refereed) Published
    Abstract [en]

    Low temperature aqueous chemical synthesis (LT-ACS) of zinc oxide (ZnO) nanorods (NRs) has been attracting considerable research interest due to its great potential in the development of light-emitting diodes (LEDs). The influence of the molar ratio of the zinc acetate (ZnAc): KOH as a ZnO seed layer precursor on the density of interface defects and hence the presence of non-radiative recombination centers in LT-ACS of ZnO NRs/GaN LEDs has been systematically investigated. The material quality of the as-prepared seed layer as quantitatively deduced by the X-ray photoelectron spectroscopy is found to be influenced by the molar ratio. It is revealed by spatially resolved cathodoluminescence that the seed layer molar ratio plays a significant role in the formation and the density of defects at the n-ZnO NRs/p-GaN heterostructure interface. Consequently, LED devices processed using ZnO NRs synthesized with molar ratio of 1:5M exhibit stronger yellow emission (similar to 575 nm) compared to those based on 1:1 and 1:3M ratios as measured by the electroluminescence. Furthermore, seed layer molar ratio shows a quantitative dependence of the non-radiative defect densities as deduced from light-output current characteristics analysis. These results have implications on the development of high-efficiency ZnO-based LEDs and may also be helpful in understanding the effects of the ZnO seed layer on defect-related non-radiative recombination. Published by AIP Publishing.

    Place, publisher, year, edition, pages
    AMER INST PHYSICS, 2016
    National Category
    Materials Chemistry
    Identifiers
    urn:nbn:se:liu:diva-129174 (URN)10.1063/1.4947593 (DOI)000375929900043 ()
    Note

    Funding Agencies|Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University (Faculty Grant SFO-Mat-LiU) [2009-00971]

    Available from: 2016-06-13 Created: 2016-06-13 Last updated: 2017-11-28
    3. Seed layer synthesis effect on the concentration of interface defects and emission spectra of ZnO nanorods/p-GaN light-emitting diode
    Open this publication in new window or tab >>Seed layer synthesis effect on the concentration of interface defects and emission spectra of ZnO nanorods/p-GaN light-emitting diode
    2017 (English)In: Physica Status Solidi (a) applications and materials science, ISSN 1862-6300, E-ISSN 1862-6319, Vol. 214, no 1, article id 1600333Article in journal (Refereed) Published
    Abstract [en]

    As the low-temperature aqueous chemical synthesis (LT-ACS), holds great promises for the synthesis of one-dimensional (1D) ZnO nanostructure-based light-emitting diodes (LEDs) and hence require parameter tuning for optimal performance. N-ZnO nanorods (NRs)/p-GaN heterojunction LEDs have been synthesized by the LT-ACS using ZnO nanoparticle (NPs) seed layers prepared with different precursor solutions. The effect of these seed layers on the interface defect properties and emission intensity of the as-synthesized n-Zn/p-GaN heterojunction LEDs has been demonstrated by spatially resolved cathodoluminescence (CL) and electroluminescence (EL) measurements, respectively. A significant reduction of the interface defects in the n-ZnO NRs/p-GaN heterostructure synthesized from a seed layer prepared from zinc acetate (ZnAc) with a mixture of potassium hydroxide (KOH) and hexamethylenetetramine (HMTA) (donated as ZKH seed) compared with those prepared from ZnAc and KOH (donated as ZK seed) is observed as revealed by spatially resolved CL. Consequently, the LEDs based on n-ZnO NRs/p-GaN prepared from ZKH seed show an improvement in the yellow emission (approximate to 578nm) compared to that based on the ZK seed as deduced from the electroluminescence measurements. The improvement in the yellow EL emission on the ZKH LED probably attributed to the low presence of the non-radiative defect as deduced by light-output current (L-I) characteristics analysis.

    Place, publisher, year, edition, pages
    WILEY-V C H VERLAG GMBH, 2017
    Keywords
    GaN; interface defects; light-emitting diodes; low-temperature aqueous chemical synthesis; seed layers; ZnO
    National Category
    Condensed Matter Physics
    Identifiers
    urn:nbn:se:liu:diva-136230 (URN)10.1002/pssa.201600333 (DOI)000394423400006 ()
    Note

    Funding Agencies|Swedish Government Strategic Research Area in Materials Science on Functional Materials (Faculty Grant SFO-Mat-LiU) at Linkoping University [2009-00971]

    Available from: 2017-03-31 Created: 2017-03-31 Last updated: 2017-11-29
    4. EPR investigation of pure and Co-doped ZnO oriented nanocrystals
    Open this publication in new window or tab >>EPR investigation of pure and Co-doped ZnO oriented nanocrystals
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    2017 (English)In: NANOTECHNOLOGY, ISSN 0957-4484, Vol. 28, no 3, article id 035705Article in journal (Refereed) Published
    Abstract [en]

    Pure and cobalt-doped zinc oxide aligned nanorods have been grown by the low-temperature (90 degrees C) aqueous chemical method on amorphous ZnO seed layer, deposited on a sapphire substrate. High crystallinity of these objects is demonstrated by the electron paramagnetic resonance investigation at liquid helium temperature. The successful incorporation of Co2+ ions in substitution of Zn2+ ones in the ZnO matrix has also been confirmed. A drastic reduction of intrinsic ZnO nanorods core defects is observed in the Co-doped samples, which enhances the structural quality of the NRs. The quantification of substitutional Co2+ ions in the ZnO matrix is achieved by comparison with a reference sample. The findings in this study indicate the potential of using the low-temperature aqueous chemical approach for synthesizing material for spintronics applications.

    Place, publisher, year, edition, pages
    IOP PUBLISHING LTD, 2017
    Keywords
    nanorods; magnetic properties; electron paramagnetic resonance; diluted magnetic semiconductors
    National Category
    Materials Chemistry
    Identifiers
    urn:nbn:se:liu:diva-134300 (URN)10.1088/1361-6528/28/3/035705 (DOI)000391289300001 ()27966469 (PubMedID)
    Note

    Funding Agencies|NATO project [SfP 984735]

    Available from: 2017-02-06 Created: 2017-02-03 Last updated: 2017-10-06
    5. An effective low-temperature solution synthesis of Co-doped [0001]-oriented ZnO nanorods
    Open this publication in new window or tab >>An effective low-temperature solution synthesis of Co-doped [0001]-oriented ZnO nanorods
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    2017 (English)In: Journal of Applied Physics, ISSN 0021-8979, E-ISSN 1089-7550, Vol. 121, no 21, article id 215102Article in journal (Refereed) Published
    Abstract [en]

    We demonstrate an efficient possibility to synthesize vertically aligned pure zinc oxide (ZnO) and Co-doped ZnO nanorods (NRs) using the low-temperature aqueous chemical synthesis (90 degrees C). Two different mixing methods of the synthesis solutions were investigated for the Co-doped samples. The synthesized samples were compared to pure ZnO NRs regarding the Co incorporation and crystal quality. Electron paramagnetic resonance (EPR) measurements confirmed the substitution of Co2+ inside the ZnO NRs, giving a highly anisotropic magnetic Co2+ signal. The substitution of Zn2+ by Co2+ was observed to be combined with a drastic reduction in the core-defect (CD) signal (g similar to 1.956) which is seen in pure ZnO NRs. As revealed by the cathodoluminescence (CL), the incorporation of Co causes a slight red-shift of the UV peak position combined with an enhancement in the intensity of the defect-related yellow-orange emission compared to pure ZnO NRs. Furthermore, the EPR and the CL measurements allow a possible model of the defect configuration in the samples. It is proposed that the as-synthesized pure ZnO NRs likely contain Zn interstitial (Zn-i(+)) as CDs and oxygen vacancy (V-O) or oxygen interstitial (O-i) as surface defects. As a result, Co was found to likely occupy the Zn-i(+), leading to the observed CDs reduction and hence enhancing the crystal quality. These results open the possibility of synthesis of highly crystalline quality ZnO NRs-based diluted magnetic semiconductors using the low-temperature aqueous chemical method. Published by AIP Publishing.

    Place, publisher, year, edition, pages
    AMER INST PHYSICS, 2017
    National Category
    Condensed Matter Physics
    Identifiers
    urn:nbn:se:liu:diva-138890 (URN)10.1063/1.4984314 (DOI)000402768900026 ()
    Note

    Funding Agencies|NATO [984735]

    Available from: 2017-06-27 Created: 2017-06-27 Last updated: 2017-10-06
    6. Core-defect reduction in ZnO nanorods by cobalt incorporation
    Open this publication in new window or tab >>Core-defect reduction in ZnO nanorods by cobalt incorporation
    Show others...
    2017 (English)In: Nanotechnology, ISSN 0957-4484, E-ISSN 1361-6528, Vol. 28, no 28, article id 285705Article in journal (Refereed) Published
    Abstract [en]

    Zinc oxide (ZnO) nanorods grown by the low-temperature (90 degrees C) aqueous chemical method with different cobalt concentration within the synthesis solution (from 0% to 15%), are studied by electron paramagnetic resonance (EPR), just above the liquid helium temperature. The anisotropic spectra of substitutional Co2+ reveal a high crystalline quality and orientation of the NRs, as well as the probable presence of a secondary disordered phase of ZnO: Co. The analysis of the EPR spectra indicates that the disappearance of the paramagnetic native core-defect (CD) at g similar to 1.96 is correlated with the apparition of the Co2+ ions lines, suggesting a gradual neutralization of the former by the latter. We show that only a little amount of cobalt in the synthesis solution (about 0.2%) is necessary to suppress almost all these paramagnetic CDs. This gives insight in the experimentally observed improvement of the crystal quality of diluted ZnO: Co nanorods, as well as into the control of paramagnetic defects in ZnO nanostructures.

    Place, publisher, year, edition, pages
    IOP PUBLISHING LTD, 2017
    Keywords
    nanorods; ZnO; physics defects; electron paramagnetic resonance
    National Category
    Condensed Matter Physics
    Identifiers
    urn:nbn:se:liu:diva-139388 (URN)10.1088/1361-6528/aa716a (DOI)000404344400005 ()28475103 (PubMedID)
    Note

    Funding Agencies|NATO project Science for Peace (SfP), Novel nanostructures [984735]

    Available from: 2017-08-07 Created: 2017-08-07 Last updated: 2017-10-06
  • 11.
    Alnoor, Hatim
    et al.
    Linköping University, Department of Science and Technology. Linköping University, Faculty of Science & Engineering.
    Pozina, Galia
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Khranovskyy, Volodymyr
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Liu, Xianjie
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Iandolo, Donata
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Willander, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Nur, Omer
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Influence of ZnO seed layer precursor molar ratio on the density of interface defects in low temperature aqueous chemically synthesized ZnO nanorods/GaN light-emitting diodes2016In: Journal of Applied Physics, ISSN 0021-8979, E-ISSN 1089-7550, Vol. 119, no 16, p. 165702-Article in journal (Refereed)
    Abstract [en]

    Low temperature aqueous chemical synthesis (LT-ACS) of zinc oxide (ZnO) nanorods (NRs) has been attracting considerable research interest due to its great potential in the development of light-emitting diodes (LEDs). The influence of the molar ratio of the zinc acetate (ZnAc): KOH as a ZnO seed layer precursor on the density of interface defects and hence the presence of non-radiative recombination centers in LT-ACS of ZnO NRs/GaN LEDs has been systematically investigated. The material quality of the as-prepared seed layer as quantitatively deduced by the X-ray photoelectron spectroscopy is found to be influenced by the molar ratio. It is revealed by spatially resolved cathodoluminescence that the seed layer molar ratio plays a significant role in the formation and the density of defects at the n-ZnO NRs/p-GaN heterostructure interface. Consequently, LED devices processed using ZnO NRs synthesized with molar ratio of 1:5M exhibit stronger yellow emission (similar to 575 nm) compared to those based on 1:1 and 1:3M ratios as measured by the electroluminescence. Furthermore, seed layer molar ratio shows a quantitative dependence of the non-radiative defect densities as deduced from light-output current characteristics analysis. These results have implications on the development of high-efficiency ZnO-based LEDs and may also be helpful in understanding the effects of the ZnO seed layer on defect-related non-radiative recombination. Published by AIP Publishing.

  • 12.
    Anwar, Nargis
    et al.
    Dundalk Inst Technol, Ireland.
    Armstrong, Gordon
    Univ Limerick, Ireland.
    Laffir, Fathima
    Univ Limerick, Ireland.
    Dickinson, Calum
    Univ Limerick, Ireland.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering.
    McCormac, Timothy
    Dundalk Inst Technol, Ireland.
    Redox switching of polyoxometalate-doped polypyrrole films in ionic liquid media2018In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 265, p. 254-258Article in journal (Refereed)
    Abstract [en]

    The surface immobilization of the parent Dawson polyoxometalate (POM) as a counter-ion for the electropolymerization of polypyrrole (PPy) or as an electrode-adhered solid was utilized for voltammetric studies of the surface adhered POM in room temperature ionic liquids (RTIL). Illustrating the efficiency of intermediate stabilization, voltammetry at POM-modified electrodes in a PF6-based RTIL revealed richer redox behaviour and higher stabilization in comparison with aqueous electrolytes and with BF4-based RTIL, respectively. High stability of the POM-doped PPy towards continuous charge-discharge voltammetric redox cycles was confirmed by minor changes in film morphology observed after the cycling in RTILs. (c) 2017 Elsevier Ltd. All rights reserved.

    The full text will be freely available from 2019-12-15 13:11
  • 13.
    Ao, Xiang
    et al.
    Huazhong University of Science and Technology, Peoples R China.
    Jiang, Jianjun
    Huazhong University of Science and Technology, Peoples R China.
    Ruan, Yunjun
    Huazhong University of Science and Technology, Peoples R China.
    Li, Zhishan
    Huazhong University of Science and Technology, Peoples R China.
    Zhang, Yi
    Wuhan Institute Technology, Peoples R China.
    Sun, Jianwu
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Wang, Chundong
    Huazhong University of Science and Technology, Peoples R China; Chinese Academic Science, Peoples R China.
    Honeycomb-inspired design of ultrafine SnO2@C nanospheres embedded in carbon film as anode materials for high performance lithium- and sodium-ion battery2017In: Journal of Power Sources, ISSN 0378-7753, E-ISSN 1873-2755, Vol. 359, p. 340-348Article in journal (Refereed)
    Abstract [en]

    Tin oxide (SnO2) has been considered as one of the most promising anodes for advanced rechargeable batteries due to its advantages such as high energy density, earth abundance and environmental friendly. However, its large volume change during the Li-Sn/Na-Sn alloying and de-alloying processes will result in a fast capacity degradation over a long term cycling. To solve this issue, in this work we design and synthesize a novel honeycomb-like composite composing of carbon encapsulated SnO2 nanospheres embedded in carbon film by using dual templates of SiO2 and NaCl. Using these composites as anodes both in lithium ion batteries and sodium-ion batteries, no discernable capacity degradation is observed over hundreds of long term cycles at both low current density (100 mA g(-1)) and high current density (500 mA g(-1)). Such a good cyclic stability and high delivered capacity have been attributed to the high conductivity of the supported carbon film and hollow encapsulated carbon shells, which not only provide enough space to accommodate the volume expansion but also prevent further aggregation of SnO2 nanoparticles upon cycling. By engineering electrodes of accommodating high volume expansion, we demonstrate a prototype to achieve high performance batteries, especially high-power batteries. (C) 2017 Elsevier B.V. All rights reserved.

  • 14.
    Arain, Munazza
    et al.
    University of Sindh, Pakistan.
    Nafady, Ayman
    King Saud University, Saudi Arabia; Sohag University, Egypt.
    Sirajuddin,
    Univ Sindh, Pakistan.
    Ibupoto, ZH
    Univ Sindh, Pakistan.
    Sherazi, Syed Tufail Hussain
    University of Sindh, Pakistan.
    Shaikh, Tayyaba
    University of Sindh, Pakistan.
    Khan, Hamayun
    Islamia Coll University, Pakistan.
    Alsalme, Ali
    King Saud University, Saudi Arabia.
    Niaz, Abdul
    Bannu University of Science and Technology, Pakistan.
    Willander, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Simpler and highly sensitive enzyme-free sensing of urea via NiO nanostructures modified electrode2016In: RSC Advances, ISSN 2046-2069, E-ISSN 2046-2069, Vol. 6, no 45, p. 39001-39006Article in journal (Refereed)
    Abstract [en]

    In this study, NiO nanostructures were synthesized via a hydrothermal process using ascorbic acid as doping agent in the presence of ammonia. As prepared nanostructures were characterized using Scanning Electron Microscopy (SEM), X-Ray Diffraction (XRD), Brunauer-Emmett-Teller (BET) specific surface area analysis, and thermogravimetric analysis (TGA). These analyses showed that these nanostructures are in the form of cotton-like porous material and crystalline in nature. Furthermore, the average size of these NiO crystallites was estimated to be 3.8 nm. These nanostructures were investigated for their potential to be a highly sensitive and selective enzyme-free sensor for detection of urea after immobilizing on a glassy carbon electrode (GCE) using 0.1% Nafion as binder. The response of this as developed amperometric sensor was linear in the range of 100-1100 mu M urea with a R-2 value of 0.990 and limit of detection (LOD) of 10 mu M. The sensor responded negligibly to various interfering species including glucose, uric acid, and ascorbic acid. This sensor was applied successfully for determining urea in real water samples such as mineral water, tap water, and river water with acceptable recovery.

  • 15.
    Armakavicius, Nerijus
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Free charge carrier properties in group III nitrides and graphene studied by THz-to-MIR ellipsometry and optical Hall effect2019Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Development of silicon based electronics have revolutionized our every day life during the last five decades. Nowadays silicon based devices operate close to their theoretical limits that is becoming a bottleneck for further progress. In particular, for the growing field of high frequency and high power electronics, silicon cannot offer the required properties. Development of materials capable of providing high current densities, carrier mobilities and high breakdown fields is crucial for further progress in state of the art electronics.

    Epitaxial graphene grown on semi-insulating silicon carbide substrates has a high potential to be integrated in current planar device technologies. High electron mobilities and sheet carrier densities make graphene extremely attractive for high frequency analog applications. One of the remaining challenges is the interaction of epitaxial graphene with the substrate. Typically, much lower free charge carrier mobilities, compared to free standing graphene, and doping, due to charge transfer from the substrate, is reported. Thus, a good understanding of the intrinsic free charge carriers properties and the factors affecting them is very important for further development of epitaxial graphene.

    Group III-nitrides have been extensively studied and already have proven their high efficiency as light emitting diodes for short wavelengths. High carrier mobilities and breakdown electric fields were demonstrated for group III-nitrides, making them attractive for high frequency and high power applications. Currently, In-rich InGaN alloys and AlGaN/GaN high electron mobility structures are of high interest for the research community due to open fundamental questions such as free charge carrier properties at high temperatures and wavefunction hybridization in AlGaN/GaN heterostructures.

    Electrical characterization techniques, commonly used for the determination of free charge carrier properties, require good ohmic and Schottky contacts, which in certain cases can be difficult to achieve. Access to electrical properties of buried conductive channels in multilayered structures requires modification of samples and good knowledge of the electrical properties of all electrical junctions within the structure. Moreover, the use of contacts to electrically characterize two-dimensional electronic materials, such as graphene, can alter their intrinsic properties. Furthermore, the determination of effective mass parameters commonly employs cyclotron resonance and Shubnikov-de Haas oscillations measurements, which require long scattering times of free charge carriers, high magnetic fields and low temperatures.

    The optical Hall effect is an external magnetic-field induced birefringence of conductive layers due to the free charge carriers interaction with long-wavelength electromagnetic waves under the influence of the Lorentz force. The optical Hall effect can be measured by generalized ellipsometry and provides a powerful method for the determination of free charge carrier properties in a non-destructive and contactless manner. The optical Hall effect measurements can provide quantitative information about free charge carrier type, concentration, mobility and effective mass parameters at temperatures ranging from few kelvins to room temperature and above. It further allows to differentiate the free charge carrier properties of individual layers in multilayer samples. The employment of a backside cavity for transparent samples can enhance the optical Hall effect and allows to access free charge carrier properties at relatively low magnetic fields using permanent magnet.

    The optical Hall effect measurements at mid-infrared spectral range can be used to probe quantum mechanical phenomena such as Landau levels in graphene. The magnetic field dependence of the inter-Landau level transition energies and optical polarization selection rules provide information about coupling properties between graphene layers and the electronic band structure.

    Measurement of the optical Hall effect by generalized ellipsometry is an indirect technique requiring subsequent data analysis. Parameterized optical models are fitted to match experimentally measured ellipsometric spectra by varying physically significant model parameters. Analysis of the generalized ellipsometry data at long wavelengths for samples containing free charge carriers by optical models based on the classical Drude formulation, augmented with an external magnetic field contribution, allows to extract carrier concentration, mobility and effective mass parameters.

    The development of the integrated FIR and THz frequency-domain ellipsometer at the Terahertz Materials Analysis Center in Linköping University was part of the graduate studies presented in this dissertation. The THz ellipsometer capabilities are demonstrated by determination of Si and sapphire optical constants, and free charge carrier properties of two-dimensional electron gas in GaN-based high electron mobility transistor structures. The THz ellipsometry is further shown to be capable of determining free charge carrier properties and following their changes upon variation of ambient conditions in atomically thin layers with an example of epitaxial graphene.

    A potential of the THz OHE with the cavity enhancement (THz-CE-OHE) for determination of the free charge carrier properties in atomically thin layers were demonstrated by the measurements of the carrier properties in monolayer and multilayer epitaxial graphene on Si-face 4H-SiC. The data analysis revealed p-type doping for monolayer graphene with a carrier density in the low 1012 cm-2 range and a carrier mobility of 1550 cm2V-1s-1. For the multilayer graphene, n-type doping with a carrier density in the low 1013 cm-2 range, a mobility of 470 cm2V-1s-1 and an effective mass of (0.14 ± 0.03)m0 were extracted. Different type of doping among monolayer and multilayer graphene is explained as a result of different hydrophobicity among samples.

    Further, we have employed THz-CE-OHE to determine for the first time anisotropic mobility parameter in quasi-free-standing bilayer epitaxial graphene induced by step-like surface morphology of 4H-SiC. Correlation of atomic force microscopy, Raman scattering spectroscopy, scanning probe Kelvin probe microscopy, low energy electron microscopy and diffraction analysis allows us to investigate the possible scattering mechanisms and suggests that anisotropic mobility is induced by varying local mobility parameter due to interaction between graphene and underlaying substrate.

    The origin of the layers decoupling in multilayer graphene on C-face 4H-SiC was studied by MIR-OHE, transmission electron microscopy and electron energy loss spectroscopy. The results revealed the decoupling of the layers induced by the increased interlayer spacing which is attributed to the Si atoms trapped between graphene layers.

    MIR ellipsometry and MIR-OHE measurements were employed to determine the electron effective mass in a wurtzite In0.33Ga0.67N epitaxial layer. The data analysis revealed the effective mass parameters parallel and perpendicular to the c-axis which can be considered as equal within sensitivity of our measurements. The determined effective mass is consistent with linear dependence on the In content.

    Analysis of the free charge carrier properties in AlGaN/GaN high electron mobility structures with modified interfaces showed that AlGaN/GaN interface structure has a significant effect on the mobility parameter. A sample with a sharp interface layers exhibits a record mobility of 2332 ± 73 cm2V-1s-1. The determined effective mass parameters showed an increase compared to the bulk GaN value, which is attributed to the penetration of the electron wavefunction into the AlGaN barrier layer.

    Temperature dependence of free charge carrier properties in GaN-based high electron mobility transistor structures with AlGaN and InAlN barrier layers were measured by terahertz optical Hall effect technique in a temperature range from 7.2 K to 398 K. The results revealed strong changes in the effective mass and mobility parameters. At temperatures below 57 K very high carrier mobility parameters above 20000 cm2V-1s-1 for AlGaN-barrier sample and much lower mobilities of ~ 5000 cm2V-1s-1 for InAlN-barrier sample were obtained. At low temperatures the effective mass parameters for both samples are very similar to bulk GaN value, while at temperatures above 131 K effective mass shows a strong increase with temperature. The effective masses of 0.344 m0 (@370 K) and 0.439 m0 (@398 K) were obtained for AlGaN- and InAlN-barrier samples, respectively. We discussed the possible origins of effective mass enhancement in high electron mobility transistor structures.  

    List of papers
    1. Advanced Terahertz Frequency-Domain Ellipsometry Instrumentation for In Situ and Ex Situ Applications
    Open this publication in new window or tab >>Advanced Terahertz Frequency-Domain Ellipsometry Instrumentation for In Situ and Ex Situ Applications
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    2018 (English)In: IEEE Transactions on Terahertz Science and Technology, ISSN 2156-342X, Vol. 8, no 3, p. 257-270Article in journal (Refereed) Published
    Abstract [en]

    We present a terahertz (THz) frequency-domain spectroscopic ellipsometer design that suppresses formation of standing waves by use of stealth technology approaches. The strategy to suppress standing waves consists of three elements geometry, coating, and modulation. The instrument is based on the rotating analyzer ellipsometer principle and can incorporate various sample compartments, such as a superconducting magnet, in situ gas cells, or resonant sample cavities, for example. A backward wave oscillator and three detectors are employed, which permit operation in the spectral range of 0.1–1 THz (3.3–33 cm−1 or 0.4–4 meV). The THz frequency-domain ellipsometer allows for standard and generalized ellipsometry at variable angles of incidence in both reflection and transmission configurations. The methods used to suppress standing waves and strategies for an accurate frequency calibration are presented. Experimental results from dielectric constant determination in anisotropic materials, and free charge carrier determination in optical Hall effect (OHE), resonant-cavity enhanced OHE, and in situ OHE experiments are discussed. Examples include silicon and sapphire optical constants, free charge carrier properties of two-dimensional electron gas in a group III nitride high electron mobility transistor structure, and ambient effects on free electron mobility and density in epitaxial graphene.

    Place, publisher, year, edition, pages
    Institute of Electrical and Electronics Engineers (IEEE), 2018
    Keywords
    Ellipsometry, Frequency-domain analysis, Instruments, Measurement by laser beam, Coherence, Dielectrics, Laser beams
    National Category
    Electrical Engineering, Electronic Engineering, Information Engineering
    Identifiers
    urn:nbn:se:liu:diva-147883 (URN)10.1109/TTHZ.2018.2814347 (DOI)000431446900001 ()2-s2.0-85045191738 (Scopus ID)
    Note

    Funding agencies: Swedish Foundation for Strategic Research (SSF) [FFL12-0181, RIF14-055]; AForsk [13-318]; Swedish Research Council (VR) [2013-5580, 2016-00889]; Swedish Governmental Agency for Innovation Systems (VINNOVA Grant) [2011-03486]; Swedish Government Strategic 

    Available from: 2018-05-18 Created: 2018-05-18 Last updated: 2019-03-05Bibliographically approved
    2. Cavity-enhanced optical Hall effect in epitaxial graphene detected at terahertz frequencies
    Open this publication in new window or tab >>Cavity-enhanced optical Hall effect in epitaxial graphene detected at terahertz frequencies
    Show others...
    2017 (English)In: Applied Surface Science, ISSN 0169-4332, E-ISSN 1873-5584, Vol. 421, p. 357-360Article in journal (Refereed) Published
    Abstract [en]

    Cavity-enhanced optical Hall effect at terahertz (THz) frequencies is employed to determine the free charge carrier properties in epitaxial graphene (EG) with different number of layers grown by high-temperature sublimation on 4H-SiC(0001). We find that one monolayer (ML) EG possesses p-type conductivity with a free hole concentration in the low 1012 cmᅵᅵᅵ2 range and a free hole mobility parameter as high as 1550 cm2/Vs. We also find that 6 ML EG shows n-type doping behavior with a much lower free electron mobility parameter of 470 cm2/Vs and an order of magnitude higher free electron density in the low 1013 cmᅵᅵᅵ2 range. The observed differences are discussed. The cavity-enhanced THz optical Hall effect is demonstrated to be an excellent tool for contactless access to the type of free charge carriers and their properties in two-dimensional materials such as EG.

    Place, publisher, year, edition, pages
    Elsevier, 2017
    Keywords
    THz optical Hall effect, Epitaxial graphene, Free charge carrier properties
    National Category
    Physical Sciences Condensed Matter Physics Atom and Molecular Physics and Optics Ceramics
    Identifiers
    urn:nbn:se:liu:diva-132407 (URN)10.1016/j.apsusc.2016.10.023 (DOI)000408756700015 ()
    Note

    Funding agencies: Swedish Research Council (VR) [2013-5580]; Swedish Governmental Agency for Innovation Systems (VINNOVA) under the VINNMER international qualification program [2011-03486, 2014-04712]; Swedish foundation for strategic research (SSF) [FFL12-0181, RIF14-055]

    Available from: 2016-11-09 Created: 2016-11-09 Last updated: 2019-03-05Bibliographically approved
    3. Electron effective mass in In0.33Ga0.67N determined by mid-infrared optical Hall effect
    Open this publication in new window or tab >>Electron effective mass in In0.33Ga0.67N determined by mid-infrared optical Hall effect
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    2018 (English)In: Applied Physics Letters, ISSN 0003-6951, E-ISSN 1077-3118, Vol. 112, no 8, article id 082103Article in journal (Refereed) Published
    Abstract [en]

    Mid-infrared optical Hall effect measurements are used to determine the free charge carrier parameters of an unintentionally doped wurtzite-structure c-plane oriented In0.33Ga0.67N epitaxial layer. Room temperature electron effective mass parameters of m(perpendicular to)* = (0.205 +/- 0.013) m(0) and m(parallel to)* = (0.204 +/- 0.016) m(0) for polarization perpendicular and parallel to the c-axis, respectively, were determined. The free electron concentration was obtained as (1.7 +/- 0.2) x 10(19) cm(-3). Within our uncertainty limits, we detect no anisotropy for the electron effective mass parameter and we estimate the upper limit of the possible effective mass anisotropy as 7%. We discuss the influence of conduction band nonparabolicity on the electron effective mass parameter as a function of In content. The effective mass parameter is consistent with a linear interpolation scheme between the conduction band mass parameters in GaN and InN when the strong nonparabolicity in InN is included. The In0.33Ga0.67N electron mobility parameter was found to be anisotropic, supporting previous experimental findings for wurtzite-structure GaN, InN, and AlxGa1-xN epitaxial layers with c-plane growth orientation. Published by AIP Publishing.

    Place, publisher, year, edition, pages
    AMER INST PHYSICS, 2018
    National Category
    Condensed Matter Physics
    Identifiers
    urn:nbn:se:liu:diva-145763 (URN)10.1063/1.5018247 (DOI)000425977500010 ()
    Note

    Funding Agencies|Swedish Governmental Agency for Innovation Systems (VINNOVA) under the VINNMER international qualification program [2011-03486]; Swedish Research Council (VR) [2016-00889]; Competence Center Program [2016-05190]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University, Faculty Grant SFO Mat LiU [2009-00971]; University of Nebraska-Lincoln; Swedish Foundation for Strategic Research (SSF) [FL12-0181, RIF14-055, EM16-0024]; J. A. Woollam Foundation; J. A. Woollam Co., Inc.; National Science Foundation [MRSEC DMR 1420645, CMMI 1337856, EAR 1521428]

    Available from: 2018-03-22 Created: 2018-03-22 Last updated: 2019-03-05
    4. Properties of two-dimensional electron gas in AlGaN/GaN HEMT structures determined by cavity-enhanced THz optical Hall effect
    Open this publication in new window or tab >>Properties of two-dimensional electron gas in AlGaN/GaN HEMT structures determined by cavity-enhanced THz optical Hall effect
    Show others...
    2016 (English)In: Physica Status Solidi C-Current Topics in Solid State Physics, Vol 13 No 5-6, Wiley-VCH Verlagsgesellschaft, 2016, Vol. 13, no 5-6, p. 369-373Conference paper, Published paper (Refereed)
    Abstract [en]

    In this work we employ terahertz (THz) ellipsometry to determine two-dimensional electron gas (2DEG) density, mobility and effective mass in AlGaN/GaN high electron mobility transistor structures grown on 4H-SiC substrates. The effect of the GaN interface exposure to low-flow-rate trimethylaluminum (TMA) on the 2DEG properties is studied. The 2DEG effective mass and sheet density are determined tobe in the range of 0.30-0.32m0 and 4.3-5.5×1012 cm–2, respectively. The 2DEG effective mass parameters are found to be higher than the bulk effective mass of GaN, which is discussed in view of 2DEG confinement. It is shown that exposure to TMA flow improves the 2DEG mobility from 2000 cm2/Vs to values above 2200 cm2/Vs. A record mobility of 2332±61 cm2/Vs is determined for the sample with GaN interface exposed to TMA for 30 s. This improvement in mobility is suggested to be due to AlGaN/GaN interface sharpening causing the reduction of interface roughness scattering of electrons in the 2DEG.

    Place, publisher, year, edition, pages
    Wiley-VCH Verlagsgesellschaft, 2016
    Series
    Physica Status Solidi C-Current Topics in Solid State Physics, ISSN 1862-6351
    Keywords
    AlGaN/GaN HEMTs, THz ellipsometry, 2DEG properties, THz optical Hall effect
    National Category
    Condensed Matter Physics
    Identifiers
    urn:nbn:se:liu:diva-133135 (URN)10.1002/pssc.201510214 (DOI)000387957200045 ()
    Conference
    11th International Conference on Nitride Semiconductors (ICNS), Beijing, China, August 30-September 4. 2015
    Available from: 2016-12-12 Created: 2016-12-09 Last updated: 2019-03-05Bibliographically approved
  • 16.
    Armakavicius, Nerijus
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Study of novel electronic materials by mid-infrared and terahertz optical Hall effect2017Licentiate thesis, comprehensive summary (Other academic)
    Abstract [en]

    Development of silicon based electronics have revolutionized our every day life during the last three decades. Nowadays Si based devices operate close to their theoretical limits that is becoming a bottleneck for further progress. In particular, for the growing field of high frequency and high power electronics, Si cannot offer the required properties. Development of materials capable of providing high current densities, carrier mobilities and high breakdown fields is crucial for a progress in state of the art electronics.

    Epitaxial graphene grown on semi-insulating silicon carbide substrates has a high potential to be integrated in the current planar device technologies. High electron mobilities and sheet carrier densities make graphene extremely attractive for high frequency analog applications. One of the remaining challenges is the interaction of epitaxial graphene with the substrate. Typically, much lower free charge carrier mobilities, compared to free standing graphene, and doping, due to charge transfer from the substrate, is reported. Thus, a good understanding of the intrinsic free charge carriers properties and the factors affecting them is very important for further development of epitaxial graphene.

    III-group nitrides have been extensively studied and already have proven their high efficiency as light sources for short wavelengths. High carrier mobilities and breakdown electric fields were demonstrated for III-group nitrides, making them attractive for high frequency and high power applications. Currently, In-rich InGaN alloys and AlGaN/GaN high electron mobility structures are of high interest for the research community due to open fundamental questions.

    Electrical characterization techniques, commonly used for the determination of free charge carrier properties, require good ohmic and Schottky contacts, which in certain cases can be difficult to achieve. Access to electrical properties of buried conductive channels in multilayered structures requires modification of samples and good knowledge of the electrical properties of all electrical contact within the structure. Moreover, the use of electrical contacts to electrically characterize two-dimensional electronic materials, such as graphene, can alter their intrinsic properties. Furthermore, the determination of effective mass parameters commonly employs cyclotron resonance and Shubnikov-de Haas oscillations measurements, which require long scattering times of free charge carriers, high magnetic fields and low temperatures.

    The optical Hall effect is an external magnetic field induced optical anisotropy in  conductive layers due to the motion of the free charge carriers under the influence of the Lorentz force, and is equivalent to the electrical Hall effect at optical frequencies. The optical Hall effect can be measured by generalized ellipsometry and provides a powerful method for the determination of free charge carrier properties in a non-destructive and contactless manner. In principle, a single optical Hall effect measurement can provide quantitative information about free charge carrier types, concentrations, mobilities and effective mass parameters at temperatures ranging from few kelvins to room temperature and above. Further, it was demonstrated that for transparent samples, a backside cavity can be employed to enhance the optical Hall effect.

    Measurement of the optical Hall effect by generalized ellipsometry is an indirect technique requiring subsequent data analysis. Parameterized optical models are fitted to match experimentally measured ellipsometric data by varying physically significant parameters. Analysis of the optical response of samples, containing free charge carriers, employing optical models based on the classical Drude model, which is augmented with an external magnetic field contribution, provide access to the free charge carrier properties.

    The main research results of the graduate studies presented in this licentiate thesis are summarized in the five scientific papers.

    Paper I. Description of the custom-built terahertz frequency-domain spectroscopic ellipsometer at Linköping University. The terahertz ellipsometer capabilities are demonstrated by an accurate determination of the isotropic and anisotropic refractive indices of silicon and m-plane sapphire, respectively. Further, terahertz optical Hall effect measurements of an AlGaN/GaN high electron mobility structures were employed to extract the two-dimensional electron gas sheet density, mobility and effective mass parameters. Last, in-situ optical Hall effect measurement on epitaxial graphene in a gas cell with controllable environment, were used to study the effects of environmental doping on the mobility and carrier concentration.

    Paper II. Presents terahertz cavity-enhanced optical Hall measurements of the monolayer and multilayer epitaxial graphene on semi-insulating 4H-SiC (0001) substrates. The data analysis revealed p-type doping for monolayer graphene with a carrier density in the low 1012 cm−2 range and a carrier mobility of 1550 cm2/V·s. For the multilayer epitaxial graphene, n-type doping with a carrier density in the low 1013 cm−2 range, a mobility of 470 cm2/V·s and an effective mass of (0.14 ± 0.03) m0 were extracted. The measurements demonstrate that cavity-enhanced optical Hall effect measurements can be applied to study electronic properties of two-dimensional materials.

    Paper III. Terahertz cavity-enhanced optical Hall effect measurements are employed to study anisotropic transport in as-grown monolayer, quasi free-standing monolayer and quasi free-standing bilayer epitaxial graphene on semi-insulating 4H-SiC (0001) substrates. The data analysis revealed a strong anisotropy in the carrier mobilities of the quasi freestanding bilayer graphene. The anisotropy is demonstrated to be induced by carriers scattering at the step edges of the SiC, by showing that the mobility is higher along the step than across them. The scattering mechanism is discussed based on the results of the optical Hall effect, low-energy electron microscopy, low-energy electron diffraction and Raman measurements.

    Paper IV. Mid-infrared spectroscopic ellipsometry and mid-infrared optical Hall effect measurements are employed to determine the electron effective mass in an In0.33Ga0.67N epitaxial layer. The data analysis reveals slightly anisotropic effective mass and carrier mobility parameters together with the optical phonon frequencies and broadenings.

    Paper V. Terahertz cavity-enhanced optical Hall measurements are employed to study the free charge carrier properties in a set of AlGaN/GaN high electron mobility structures with modified interfaces. The results show that the interface structure has a significant effect on the free charge carrier mobility and that the sample with a sharp interface between an AlGaN barrier and a GaN buffer layers exhibits a record mobility of 2332±73 cm2/V·s. The determined effective mass parameters showed an increase compared to the GaN value, that is attributed the the penetration of the electron wavefunction into the AlGaN barrier layer.

    List of papers
    1. Cavity-enhanced optical Hall effect in epitaxial graphene detected at terahertz frequencies
    Open this publication in new window or tab >>Cavity-enhanced optical Hall effect in epitaxial graphene detected at terahertz frequencies
    Show others...
    2017 (English)In: Applied Surface Science, ISSN 0169-4332, E-ISSN 1873-5584, Vol. 421, p. 357-360Article in journal (Refereed) Published
    Abstract [en]

    Cavity-enhanced optical Hall effect at terahertz (THz) frequencies is employed to determine the free charge carrier properties in epitaxial graphene (EG) with different number of layers grown by high-temperature sublimation on 4H-SiC(0001). We find that one monolayer (ML) EG possesses p-type conductivity with a free hole concentration in the low 1012 cmᅵᅵᅵ2 range and a free hole mobility parameter as high as 1550 cm2/Vs. We also find that 6 ML EG shows n-type doping behavior with a much lower free electron mobility parameter of 470 cm2/Vs and an order of magnitude higher free electron density in the low 1013 cmᅵᅵᅵ2 range. The observed differences are discussed. The cavity-enhanced THz optical Hall effect is demonstrated to be an excellent tool for contactless access to the type of free charge carriers and their properties in two-dimensional materials such as EG.

    Place, publisher, year, edition, pages
    Elsevier, 2017
    Keywords
    THz optical Hall effect, Epitaxial graphene, Free charge carrier properties
    National Category
    Physical Sciences Condensed Matter Physics Atom and Molecular Physics and Optics Ceramics
    Identifiers
    urn:nbn:se:liu:diva-132407 (URN)10.1016/j.apsusc.2016.10.023 (DOI)000408756700015 ()
    Note

    Funding agencies: Swedish Research Council (VR) [2013-5580]; Swedish Governmental Agency for Innovation Systems (VINNOVA) under the VINNMER international qualification program [2011-03486, 2014-04712]; Swedish foundation for strategic research (SSF) [FFL12-0181, RIF14-055]

    Available from: 2016-11-09 Created: 2016-11-09 Last updated: 2019-03-05Bibliographically approved
    2. Properties of two-dimensional electron gas in AlGaN/GaN HEMT structures determined by cavity-enhanced THz optical Hall effect
    Open this publication in new window or tab >>Properties of two-dimensional electron gas in AlGaN/GaN HEMT structures determined by cavity-enhanced THz optical Hall effect
    Show others...
    2016 (English)In: Physica Status Solidi C-Current Topics in Solid State Physics, Vol 13 No 5-6, Wiley-VCH Verlagsgesellschaft, 2016, Vol. 13, no 5-6, p. 369-373Conference paper, Published paper (Refereed)
    Abstract [en]

    In this work we employ terahertz (THz) ellipsometry to determine two-dimensional electron gas (2DEG) density, mobility and effective mass in AlGaN/GaN high electron mobility transistor structures grown on 4H-SiC substrates. The effect of the GaN interface exposure to low-flow-rate trimethylaluminum (TMA) on the 2DEG properties is studied. The 2DEG effective mass and sheet density are determined tobe in the range of 0.30-0.32m0 and 4.3-5.5×1012 cm–2, respectively. The 2DEG effective mass parameters are found to be higher than the bulk effective mass of GaN, which is discussed in view of 2DEG confinement. It is shown that exposure to TMA flow improves the 2DEG mobility from 2000 cm2/Vs to values above 2200 cm2/Vs. A record mobility of 2332±61 cm2/Vs is determined for the sample with GaN interface exposed to TMA for 30 s. This improvement in mobility is suggested to be due to AlGaN/GaN interface sharpening causing the reduction of interface roughness scattering of electrons in the 2DEG.

    Place, publisher, year, edition, pages
    Wiley-VCH Verlagsgesellschaft, 2016
    Series
    Physica Status Solidi C-Current Topics in Solid State Physics, ISSN 1862-6351
    Keywords
    AlGaN/GaN HEMTs, THz ellipsometry, 2DEG properties, THz optical Hall effect
    National Category
    Condensed Matter Physics
    Identifiers
    urn:nbn:se:liu:diva-133135 (URN)10.1002/pssc.201510214 (DOI)000387957200045 ()
    Conference
    11th International Conference on Nitride Semiconductors (ICNS), Beijing, China, August 30-September 4. 2015
    Available from: 2016-12-12 Created: 2016-12-09 Last updated: 2019-03-05Bibliographically approved
  • 17.
    Ashaduzzaman, Md
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering. University of Dhaka, Bangladesh.
    Anto Antony, Aswathi
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering.
    Murugan, N. Arul
    Royal Institute Technology, Sweden.
    Deshpande, Swapneel R.
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering.
    Turner, Anthony
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering.
    Tiwari, Ashutosh
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering. Tekidag AB, UCS, S-58330 Linkoping, Sweden.
    Studies on an on/off-switchable immunosensor for troponin T2015In: Biosensors & bioelectronics, ISSN 0956-5663, E-ISSN 1873-4235, Vol. 73, p. 100-107Article in journal (Refereed)
    Abstract [en]

    Regeneration is a key goal in the design of immunosensors. In this study, we report the temperature-regulated interaction of N-isopropylacrylamide (PNIPAAm) functionalised cardiac troponin T (cTnT) with anti-cTnT. Covalently bonded PNIPAAm on an anti-cTnT bioelectrode showed on/off-switchability, regeneration capacity and temperature triggered sensitivity for cTnT. Above the lower critical solution temperature (LCST), PNIPAAm provides a liphophilic microenvironment with specific volume reduction at the bioelectrode surface, making available binding space for cTnT, and facilitating analyte recognition. Computational studies provide details about the structural changes occurring at the electrode above and below the LCST. Furthermore, free energies associated with the binding of cTnT with PNIPAAm at 25 (Delta G(coil)=-6.0 Kcal/mole) and 37 degrees C (Delta G(globular)=-41.0 kcal/mole) were calculated to elucidate the interaction and stability of the antigen-antibody complex. The responsiveness of such assemblies opens the way for miniaturised, smart immuno-technologies with built-in programmable interactions of antigen-antibody upon receiving stimuli.

  • 18.
    Asif, Muhammad
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology. COMSATS institute of Information Technology, Lahore, Pakistan.
    Elinder, Fredrik
    Linköping University, Department of Clinical and Experimental Medicine, Division of Cell Biology. Linköping University, Faculty of Health Sciences.
    Willander, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Electrochemical Biosensors Based on ZnO Nanostructures to Measure Intracellular Metal Ions and Glucose2011In: Journal of Analytical & Bioanalytical Techniques, ISSN 2155-9872, Vol. S7, no 003, p. 1-9Article in journal (Refereed)
    Abstract [en]

    Zinc oxide (ZnO) nanostructures have attracted much interest for intracellular electrochemical measurements because of its large surface area, and its biocompatible properties. To design intracellular biosensors for metal ions and glucose, we grew ZnO nanorods on the tip of borosilicate glass capillaries (0.7μm in diameter) and characterized the nano-scale structure with field-emission scanning electron microscopy and high-resolution transmission electron microscopy. The ZnO nanorods were functionalized accordingly for intracellular free metal ions or glucose measurements. Selectivity was achieved by using a metal-ion selective plastic membrane or glucose oxidase enzyme for glucose measurements. These functionalized ZnO nanorods showed high sensitivity and good biocompatibility for intracellular environments. Human adipocytes and frog oocytes were used for determinations of intracellular free metal ions and glucose concentrations. In this review, we discuss the simple and direct approach for intracellular measurements using ZnO nanostructure-based potentiometric biosensors for clinical and non-clinical applications. The performance of ZnO nanostructure-based intracellular sensor can be improved through engineering of morphology, effective surface area, functionality, and adsorption/desorption capability. This study paves the way to find applications in biomedicine by using this simple and miniaturized biosensing device

  • 19.
    Askari, Sadegh
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Plasma and Coating Physics. Linköping University, Faculty of Science & Engineering. Christian Albrechts Univ Kiel, Germany.
    Mariotti, Davide
    Ulster Univ, North Ireland.
    Stehr, Jan Eric
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Benedikt, Jan
    Christian Albrechts Univ Kiel, Germany.
    Keraudy, Julien
    Linköping University, Department of Physics, Chemistry and Biology, Plasma and Coating Physics. Linköping University, Faculty of Science & Engineering.
    Helmersson, Ulf
    Linköping University, Department of Physics, Chemistry and Biology, Plasma and Coating Physics. Linköping University, Faculty of Science & Engineering.
    Low-Loss and Tunable Localized Mid-Infrared Plasmons in Nanocrystals of Highly Degenerate InN2018In: Nano letters (Print), ISSN 1530-6984, E-ISSN 1530-6992, Vol. 18, no 9, p. 5681-5687Article in journal (Refereed)
    Abstract [en]

    Plasmonic response of free charges confined in nanostructures of plasmonic materials is a powerful means for manipulating the light-material interaction at the nanoscale and hence has influence on various relevant technologies. In particular, plasmonic materials responsive in the mid-infrared range are technologically important as the mid-infrared is home to the vibrational resonance of molecules and also thermal radiation of hot objects. However, the development of the field is practically challenged with the lack of low-loss materials supporting high quality plasmons in this range of the spectrum. Here, we demonstrate that degenerately doped InN nanocrystals (NCs) support tunable and low-loss plasmon resonance spanning the entire midwave infrared range. Modulating free-carrier concentration is achieved by engineering nitrogen-vacancy defects (InN1-x, 0.017 amp;lt; x amp;lt; 0.085) in highly degenerate NCs using a nonequilibrium gas-phase growth process. Despite the significant reduction in the carrier mobility relative to intrinsic InN, the mobility in degenerate InN NCs (amp;gt;60 cm(2)/(V s)) remains considerably higher than the carrier mobility reported for other materials NCs such as doped metal oxides, chalcogenides, and noble metals. These findings demonstrate feasibility of controlled tuning of infrared plasmon resonances in a low-loss material of III-V compounds and open a gateway to further studies of these materials nanostructures for infrared plasmonic applications.

  • 20.
    Atakan, Aylin
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Nanostructured Materials. Linköping University, Faculty of Science & Engineering.
    Mäkie, Peter
    Linköping University, Department of Physics, Chemistry and Biology, Nanostructured Materials. Linköping University, Faculty of Science & Engineering.
    Söderlind, Fredrik
    Linköping University, Department of Physics, Chemistry and Biology, Chemistry. Linköping University, Faculty of Science & Engineering.
    Keraudy, Julien
    Linköping University, Department of Physics, Chemistry and Biology, Plasma and Coating Physics. Linköping University, Faculty of Science & Engineering.
    Johansson, Emma
    Linköping University, Department of Physics, Chemistry and Biology, Nanostructured Materials. Linköping University, Faculty of Science & Engineering.
    Odén, Magnus
    Linköping University, Department of Physics, Chemistry and Biology, Nanostructured Materials. Linköping University, Faculty of Science & Engineering.
    Synthesis of a Cu-infiltrated Zr-doped SBA-15 catalyst for CO2 hydrogenation into methanol and dimethyl ethert2017In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 19, no 29, p. 19139-19149Article in journal (Refereed)
    Abstract [en]

    A catalytically active nanoassembly comprising Cu-nanoparticles grown on integrated and active supports (large pore Zr-doped mesoporous SBA-15 silica) has been synthesized and used to promote CO2 hydrogenation. The doped mesoporous material was synthesized using a sal-gel method, in which the pore size was tuned between 11 and 15 nm while maintaining a specific surface area of about 700 m(2) g (1). The subsequent Cu nanoparticle growth was achieved by an infiltration process involving attachment of different functional groups on the external and internal surfaces of the mesoporous structure such that 7-10 nm sized Cu nanoparticles grew preferentially inside the pores. Chemisorption showed improved absorption of both CO2 and H-2 for the assembly compared to pure SBA-15 and 15% of the total CO2 was converted to methanol and dimethyl ether at 250 degrees C and 33 bar.

  • 21.
    Aziz, Shazed
    et al.
    Department of Chemical and Environmental Engineering, Faculty of Engineering, University Putra Malaysia, Selangor, Malaysia.
    Rashid, Suraya
    Department of Chemical and Environmental Engineering, Faculty of Engineering, University Putra Malaysia, Selangor, Malaysia; Advanced Materials and Nanotechnology Lab , Institute of Advanced Technology, University Putra Malaysia, Selangor, Malaysia.
    Salleh, Mohamad Amran Mohd
    Department of Chemical and Environmental Engineering, Faculty of Engineering, University Putra Malaysia, Selangor, Malaysia; Advanced Materials and Nanotechnology Lab, Institute of Advanced Technology, University Putra Malaysia, Selangor, Malaysia.
    Theoretical Prediction of CNT-CF/PP Composite Tensile Properties Using Various Numerical Modeling Methods2013In: Fullerenes, nanotubes, and carbon nanostructures (Print), ISSN 1536-383X, E-ISSN 1536-4046, Vol. 21, no 5, p. 411-416Article in journal (Refereed)
    Abstract [en]

    Development of effective models to predict tensile properties of ‘carbon nanotube coated carbon fibre reinforced polypropylene (CNT-CF/PP)’ composites is briefly discussed. The composite taken as the reference is based on the highest growth mechanism of CNTs over carbon fibres. Halpin-Tsai and Combined Voigt-Reuss model has been implemented. Young's modulus for CNT-CF/PP composites has been found 4.5368 GPa and the tensile strength has been estimated 45.367 MPa considering the optimum operating condition of chemical vapor deposition (CVD) technique. Stiffness of the composite is represented through the stress-strain plots; stiffness is proportional to the steepness of the slope. There are slight deviations of results that have been found theoretically over the experimental issues.

  • 22.
    Bai, Jianhao
    et al.
    National University of Singapore.
    Beyer, Sebastian
    National University of Singapore.
    Mak, Wing Cheung
    Hong Kong University of Science and Technology, Hong Kong, China .
    Trau, Dieter
    National University of Singapore.
    Fabrication of inflated LbL microcapsules with a ‘bead-in-a-capsule’ morphology2009In: Soft Matter, ISSN 1744-683X, E-ISSN 1744-6848, Vol. 5, p. 4152-4160Article in journal (Refereed)
    Abstract [en]

    The fabrication of inflated Layer-by-Layer (LbL) microcapsules with a unique ‘bead-in-a-capsule’ morphology is presented. Currently, the fabrication of LbL microcapsules using conventional aqueous LbL techniques usually results in microcapsules with a two-phase system (LbL capsular wall with an air, liquid, solid or hydrogel core). Here, we present the fabrication of inflated LbL microcapsules with a unique three-phase system (LbL capsular wall, hydrogel microbead in an aqueous core) by using the Reverse-Phase LbL (RP-LbL) technique. The RP-LbL technique is performed in an organic solvent and allows encapsulation of water-soluble templates and molecules with high efficiency. Firstly, the RP-LbL technique is used to coat polymer layers onto agarose microbeads containing TRIS buffer for the formation of LbL capsular walls onto the microbeads and to minimize out-diffusion of encapsulated TRIS. Next, the polymer-coated agarose microbeads are transferred from an organic to an aqueous solvent where the TRIS molecules induce an osmotic pressure in the microcapsules' interior. This pressure drives the inflation of the LbL microcapsules that causes the expansion of the LbL capsular walls. Fluorescence staining reveals that the inflated LbL microcapsules consist of an agarose microbead suspended within the aqueous interior of the capsule but still attached to the LbL capsular wall at one point; thereby displaying a ‘bead-in-a-capsule’ morphology. It was demonstrated that the degree of inflation depends on the concentration of pre-loaded TRIS and the number of coated polymer layers. Also, ADOGEN® 464 (a cationic surfactant) is required for the fabrication of the inflated LbL microcapsules. The mass of dextran macromolecules (65–2000 kDa) diffusing through the LbL capsular wall had decreased by at least 49% after expansion of the capsular wall. Inflated microcapsules were shown to be capable of controlling the distribution of two different materials internally. Hence, it is possible that inflated microcapsules can permit localized control over chemical or enzymatic reactions for future uses in biomedical applications.

  • 23.
    Bai, Sai
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Yuan, Zhongcheng
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Gao, Feng
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Colloidal metal halide perovskite nanocrystals: synthesis, characterization, and applications2016In: Journal of Materials Chemistry C, ISSN 2050-7526, E-ISSN 2050-7534, Vol. 4, no 18, p. 3898-3904Article in journal (Refereed)
    Abstract [en]

    Colloidal metal halide perovskite nanocrystals (NCs) have emerged as promising materials for optoelectronic devices and received considerable attention recently. Their superior photoluminescence (PL) properties provide significant advantages for lighting and display applications. In this Highlight, we discuss recent developments in the design and chemical synthesis of colloidal perovskite NCs, including both organic-inorganic hybrid and all inorganic perovskite NCs. We review the excellent PL properties and current optoelectronic applications of these perovskite NCs. In addition, critical challenges that currently limit the applicability of perovskite NCs are discussed, and prospects for future directions are proposed.

  • 24.
    Battocchio, Chiara
    et al.
    Roma Tre Univ, Italy.
    Concolato, Sofia
    Roma Tre Univ, Italy.
    De Santis, Serena
    Roma Tre Univ, Italy.
    Fahlman, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Iucci, Giovanna
    Roma Tre Univ, Italy.
    Santi, Marta
    Roma Tre Univ, Italy.
    Sotgiu, Giovanni
    Roma Tre Univ, Italy.
    Orsini, Monica
    Roma Tre Univ, Italy.
    Chitosan functionalization of titanium and Ti6Al4V alloy with chloroacetic acid as linker agent2019In: Materials science & engineering. C, biomimetic materials, sensors and systems, ISSN 0928-4931, E-ISSN 1873-0191, Vol. 99, p. 1133-1140Article in journal (Refereed)
    Abstract [en]

    In this work, a new covalent grafting of chitosan on titanium and Ti6Al4V alloy surfaces is reported using chloroacetic acid as linker agent. Good results were obtained both on titanium and on Ti6Al4V alloy. The effect of the surface acid pretreatments on the subsequent functionalization with chitosan is evaluated. The morphological aspect of acid etched metal surfaces before chitosan grafting has been characterized by scanning electron microscopy (SEM). The presence of carboxylic groups on metal surfaces and then the efficiency of chitosan covalent immobilization were detected by Fourier transformed infrared-Attenuated Total Reflectance (FTIR-ATR) and X-Ray photoelectron spectroscopy (XPS). Cyclic voltammetry tests, using the functionalized titanium and Ti6Al4V samples as electrodes, were conducted in different aqueous solutions, to detect the presence of the homogeneous overlayer of chitosan on the surface, and to evaluate the importance of the carboxyl groups as linker agent.

  • 25.
    Bengtsson, Katarina
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Electrokinetic devices from polymeric materials2017Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    There are multiple applications for polymers: our bodies are built of them, plastic bags and boxes used for storage are composed of them, as are the shells for electronics, TVs, computers, clothes etc. Many polymers are cheap, and easy to manufacture and process which make them suitable for disposable systems. The choice of polymer to construct an object will therefore highly influence the properties of the object itself. The focus of this thesis is the application of commonly used polymers to solve some challenges regarding integration of electrodes in electrokinetic devices and 3D printing.

    The first part of this thesis regards electrokinetic systems and the electrodes’ impact on the system. Electrokinetic systems require Faradaic (electrochemical) reactions at the electrodes to maintain an electric field in an electrolyte. The electrochemical reactions at the electrodes allow electron-to-ion transduction at the electrode-electrolyte interface, necessary to drive a current at the applied potential through the system, which thereby either cause flow (electroosmosis) or separation (electrophoresis). These electrochemical reactions at the electrodes, such as water electrolysis, are usually problematic in analytical systems and systems applied in biology. One solution to reduce the impact of water electrolysis is by replacing metal electrodes with electrochemically active polymers, e.g. poly(3,4-ethylenedioxythiophene) (PEDOT). Paper 1 demonstrates that PEDOT electrodes can replace platinum electrodes in a gel electrophoretic setup. Paper 2 reports an all-plastic, planar, flexible electroosmotic pump which continuously transports water from one side to the other using potentials as low as 0.3 V. This electroosmotic pump was further developed in paper 3, where it was made into a compact and modular setup, compatible with commercial microfluidic devices. We demonstrated that the pump could maintain an alternating flow for at least 96 h, with a sufficient flow of cell medium to keep cells alive for the same period of time.

    The second part of the thesis describes the use of 3D printers for manufacturing prototypes and the material requirements for 3D printing. Protruding and over-hanging structures are more challenging to print using a 3D printer and usually require supporting material during the printing process. In paper 4, we showed that polyethylene glycol (PEG), in combination with a carbonate-based plasticizer, functions well as a 3D printable sacrificial template material. PEG2000 with between 20 and 30 wt% dimethyl carbonate or propylene carbonate have good shear-thinning rheology, mechanical and chemical stability, and water solubility, which are advantageous for a supporting material used in 3D printing.

    The advances presented in this thesis have solved some of the challenges regarding electrokinetic systems and prototype manufacturing. Hopefully this will contribute to the development of robust, disposable, low-cost, and autonomous electrokinetic devices.

    List of papers
    1. Conducting Polymer Electrodes for Gel Electrophoresis
    Open this publication in new window or tab >>Conducting Polymer Electrodes for Gel Electrophoresis
    2014 (English)In: PLoS ONE, ISSN 1932-6203, E-ISSN 1932-6203, Vol. 9, no 2, p. 0089416-Article in journal (Refereed) Published
    Abstract [en]

    In nearly all cases, electrophoresis in gels is driven via the electrolysis of water at the electrodes, where the process consumes water and produces electrochemical by-products. We have previously demonstrated that p-conjugated polymers such as poly(3,4-ethylenedioxythiophene) (PEDOT) can be placed between traditional metal electrodes and an electrolyte to mitigate electrolysis in liquid (capillary electroosmosis/electrophoresis) systems. In this report, we extend our previous result to gel electrophoresis, and show that electrodes containing PEDOT can be used with a commercial polyacrylamide gel electrophoresis system with minimal impact to the resulting gel image or the ionic transport measured during a separation.

    Place, publisher, year, edition, pages
    Public Library of Science, 2014
    National Category
    Engineering and Technology
    Identifiers
    urn:nbn:se:liu:diva-105901 (URN)10.1371/journal.pone.0089416 (DOI)000331711900141 ()
    Available from: 2014-04-14 Created: 2014-04-12 Last updated: 2017-12-05Bibliographically approved
  • 26.
    Beyer, Sebastian
    et al.
    Gelsenkirchen University of Applied Sciences, Germany.
    Mak, Wing Cheung
    National University of Singapore.
    Trau, Dieter
    National University of Singapore.
    Reverse-phase LbL-encapsulation of highly water soluble materials by layer-by-layer polyelectrolyte self-assembly2007In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 23, no 17, p. 8827-8832Article in journal (Refereed)
    Abstract [en]

    We report on a novel method for the encapsulation of highly water soluble materials by using layer-by-layer (LbL) polyelectrolyte self-assembly. State of the art polyelectrolyte self-assembly LbL coating and encapsulation methods are only applicable to insoluble or poorly water soluble template materials, because the process is performed in water causing dissolution of the solid template. Our method extends the material spectrum to highly water soluble template materials by using non-ionized polyelectrolytes in an organic phase (reverse-phase) instead of polyelectrolyte salts in an aqueous environment. By using the reverse-phase layer-by-layer (RP-LbL) technique, we have demonstrated the direct encapsulation of proteins, glucose, vitamin C, and inorganic salts in the solid state. Multilayer deposition was proven, layer thickness was determined by AFM, and the advantage of the method to prepare powders of encapsulated materials was demonstrated. The method is simple, robust, and applicable to a broad range of substances with potential applications in several industries.

  • 27.
    Björk, Emma
    Linköping University, Department of Physics, Chemistry and Biology, Nanostructured Materials. Linköping University, Faculty of Science & Engineering.
    Synthesizing and Characterizing Mesoporous Silica SBA-15: A Hands On Laboratory Experiment for Undergraduates Using Various Instrumental Techniques2017In: Journal of Chemical Education, ISSN 0021-9584, E-ISSN 1938-1328, Vol. 94, no 1, p. 91-94Article in journal (Refereed)
    Abstract [en]

    In this laboratory experiment, students learn how to synthesize mesoporous silica of the SBA-15 type and explore how the different synthesis steps affect the final material. Mesoporous materials, especially SBA-15, are often used in the development of new methods for. drug delivery, catalysis, and separation because of the flexibility of tailoring these materials to optimize the performance in different applications. However, the synthesis of mesoporous materials is rarely introduced to undergraduate students. The material synthesis is a simple sol gel process, where small alterations in the synthesis steps can significantly change the material characteristics. The presented laboratory experiment aims to introduce undergraduate students to the synthesis of SBA-15 mesoporous silica with different pore sizes due to alterations in the hydrothermal treatment time and/ or temperature and to give students hands-on experience with important characterization tools, including physisorption, X-ray diffraction, FTIR spectroscopy, and thermogravimetric analysis, to understand the effect of hydrothermal treatment and surfactant removal. Additional synthesis parameters to study, such as surfactant removal, the silica precursor, and pore swelling agents, are also presented. The experiment has been used in teaching of both bachelors and masters students and can be adapted to various instrumental techniques, e.g., scanning electron microscopy for morphology studies, transition electron microscopy for pore structure characterization, etc.

  • 28.
    Björk, Emma
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Nanostructured Materials. Linköping University, Faculty of Science & Engineering. Univ Ulm, Germany.
    Mäkie, Peter
    Linköping University, Department of Physics, Chemistry and Biology, Nanostructured Materials. Linköping University, Faculty of Science & Engineering.
    Rogström, Lina
    Linköping University, Department of Physics, Chemistry and Biology, Nanostructured Materials. Linköping University, Faculty of Science & Engineering.
    Atakan, Aylin
    Linköping University, Department of Physics, Chemistry and Biology, Nanostructured Materials. Linköping University, Faculty of Science & Engineering.
    Schell, Norbert
    Helmholtz Zentrum Geesthacht, Germany.
    Odén, Magnus
    Linköping University, Department of Physics, Chemistry and Biology, Nanostructured Materials. Linköping University, Faculty of Science & Engineering.
    Formation of block-copolymer-templated mesoporous silica2018In: Journal of Colloid and Interface Science, ISSN 0021-9797, E-ISSN 1095-7103, Vol. 521, p. 183-189Article in journal (Refereed)
    Abstract [en]

    In situ attenuated total reflectance Fourier transform infrared spectroscopy is used to monitor the chemical evolution of the mesoporous silica SBA-15 from hydrolysis of the silica precursor to final silica condensation after the particle formation. Two silica precursors, tetraethyl orthosilicate (TEOS) or sodium metasilicate (SMS) were used, and the effects of additive (heptane and NH4F) concentrations were studied. Five formation stages are identified when TEOS is used as the precursor. The fourth stage correlates with the appearance and evolution of diffraction peaks recorded using in situ small angle X-ray diffraction. Details of the formed silica matrix are observed, e.g. the ratio between six-fold cyclic silica rings and linear bonding increases with the NH4F concentration. The TEOS hydrolysis time is independent of the NH4F concentration for small amounts of heptane, but is affected by the size of the emulsion droplets when the heptane amount increases. Polymerization and condensation rates of both silica precursors are affected by the salt concentration. Materials synthesized using SMS form significantly faster compared to TEOS-materials due to the pre-hydrolysis of the precursor. The study provides detailed insights into how the composition of the synthesis solution affects the chemical evolution and micellar aggregation during formation of mesoporous silica. (C) 2018 Elsevier Inc. All rights reserved.

    The full text will be freely available from 2020-03-13 13:33
  • 29.
    Blomqvist, A
    et al.
    Sandvik Tooling.
    Århammar, Cecilia
    Uppsala University.
    Pedersen, Henrik
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
    Silvearv, Fredrik
    Uppsala University.
    Norgren, Susanne
    Sandvik Mining and Construction.
    Ahuja, R
    Uppsala University.
    Understanding the catalytic effects of H2S on CVD-growth of α-alumina: Thermodynamic gas-phase simulations and density functional theory2011In: Surface & Coatings Technology, ISSN 0257-8972, E-ISSN 1879-3347, Vol. 206, no 7, p. 1771-1779Article in journal (Refereed)
    Abstract [en]

    The catalytic effect of H2S on the AlCl3/H2/CO2/HCl chemical vapor deposition (CVD) process has been investigatedon an atomistic scale. We apply a combined approach with thermodynamic modeling and densityfunctional theory and show that H2S acts as mediator for the oxygenation of the Al-surface which will inturn increase the growth rate of Al2O3. Furthermore we suggest surface terminations for the three investigatedsurfaces. The oxygen surface is found to be hydrogenated, in agreement with a number of previous works.The aluminum surfaces are Cl-terminated in the studied CVD-process. Furthermore, we find that the AlClOmolecule is a reactive transition state molecule which interacts strongly with the aluminum and oxygensurfaces.

  • 30.
    Bouhafs, Chamseddine
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Structural and Electronic Properties of Graphene on 4H- and 3C-SiC2016Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Graphene is a one-atom-tick carbon layer arranged in a honeycomb lattice. Graphene was first experimentally demonstrated by Andre Geim and Konstantin Novoselov in 2004 using mechanical exfoliation of highly oriented pyrolytic graphite (exfoliated graphene flakes), for which they received the Nobel Prize in Physics in 2010. Exfoliated graphene flakes show outstanding electronic properties, e.g., very high free charge carrier mobility parameters and ballistic transport at room temperature. This makes graphene a suitable material for next generation radio-frequency and terahertz electronic devices. Such applications require fabrication methods of large-area graphene compatible with electronic industry. Graphene grown by sublimation on silicon carbide (SiC) offers a viable route towards production of large-area, electronic-grade material on semi-insulating substrate without the need of transfer. Despite the intense investigations in the field, uniform wafer-scale graphene with very high-quality that matches the properties of exfoliated graphene has not been achieved yet. The key point is to identify and control how the substrate affects graphene uniformity, thickness, layer stacking, structural and electronic properties. Of particular interest is to understand the effects of SiC surface polarity and polytype on graphene properties in order to achieve large-area material with tailored properties for electronic applications. The main objectives of this thesis are to address these issues by investigating the structural and electronic properties of epitaxial graphene grown on 4HSiC and 3C-SiC substrates with different surface polarities. The first part of the thesis includes a general description of the properties of graphene, bilayer graphene and graphite. Then, the properties of epitaxial graphene on SiC by sublimation are detailed. The experimental techniques used to characterize graphene are described. A summary of all papers and contribution to the field is presented at the end of Part I. Part II consists of seven papers.

    List of papers
    1. Structural properties and dielectric function of graphene grown by high-temperature sublimation on 4H-SiC(000-1)
    Open this publication in new window or tab >>Structural properties and dielectric function of graphene grown by high-temperature sublimation on 4H-SiC(000-1)
    Show others...
    2015 (English)In: Journal of Applied Physics, ISSN 0021-8979, E-ISSN 1089-7550, Vol. 117, no 8, p. 085701-Article in journal (Refereed) Published
    Abstract [en]

    Understanding and controlling growth of graphene on the carbon face (C-face) of SiC presents a significant challenge. In this work, we study the structural, vibrational, and dielectric function properties of graphene grown on the C-face of 4H-SiC by high-temperature sublimation in an argon atmosphere. The effect of growth temperature on the graphene number of layers and crystallite size is investigated and discussed in relation to graphene coverage and thickness homogeneity. An amorphous carbon layer at the interface between SiC and the graphene is identified, and its evolution with growth temperature is established. Atomic force microscopy, micro-Raman scattering spectroscopy, spectroscopic ellipsometry, and high-resolution cross-sectional transmission electron microscopy are combined to determine and correlate thickness, stacking order, dielectric function, and interface properties of graphene. The role of surface defects and growth temperature on the graphene growth mechanism and stacking is discussed, and a conclusion about the critical factors to achieve decoupled graphene layers is drawn. (C) 2015 AIP Publishing LLC.

    Place, publisher, year, edition, pages
    American Institute of Physics (AIP), 2015
    National Category
    Condensed Matter Physics
    Identifiers
    urn:nbn:se:liu:diva-117253 (URN)10.1063/1.4908216 (DOI)000351132500070 ()
    Note

    Funding Agencies|Marie Curie actions [264613-NetFISiC]; Swedish Research Council (VR) [2011-4447, 2013-5580]; Swedish Governmental Agency for Innovation Systems (VINNOVA) under the VINNMER international qualification program [2011-03486]; Swedish foundation for strategic research (SSF) [FFL12-0181]; FP7 EU project Nano-Rf [FP7-ICT-2011-8]; French ANR under the Grafonics Project [ANR-10-NANO-0004]; European Union Seventh Framework Programme under Graphene Flagship [604391]; Knut and Alice Wallenbergs foundation

    Available from: 2015-04-22 Created: 2015-04-21 Last updated: 2017-12-04
    2. Cavity-enhanced optical Hall effect in epitaxial graphene detected at terahertz frequencies
    Open this publication in new window or tab >>Cavity-enhanced optical Hall effect in epitaxial graphene detected at terahertz frequencies
    Show others...
    2017 (English)In: Applied Surface Science, ISSN 0169-4332, E-ISSN 1873-5584, Vol. 421, p. 357-360Article in journal (Refereed) Published
    Abstract [en]

    Cavity-enhanced optical Hall effect at terahertz (THz) frequencies is employed to determine the free charge carrier properties in epitaxial graphene (EG) with different number of layers grown by high-temperature sublimation on 4H-SiC(0001). We find that one monolayer (ML) EG possesses p-type conductivity with a free hole concentration in the low 1012 cmᅵᅵᅵ2 range and a free hole mobility parameter as high as 1550 cm2/Vs. We also find that 6 ML EG shows n-type doping behavior with a much lower free electron mobility parameter of 470 cm2/Vs and an order of magnitude higher free electron density in the low 1013 cmᅵᅵᅵ2 range. The observed differences are discussed. The cavity-enhanced THz optical Hall effect is demonstrated to be an excellent tool for contactless access to the type of free charge carriers and their properties in two-dimensional materials such as EG.

    Place, publisher, year, edition, pages
    Elsevier, 2017
    Keywords
    THz optical Hall effect, Epitaxial graphene, Free charge carrier properties
    National Category
    Physical Sciences Condensed Matter Physics Atom and Molecular Physics and Optics Ceramics
    Identifiers
    urn:nbn:se:liu:diva-132407 (URN)10.1016/j.apsusc.2016.10.023 (DOI)000408756700015 ()
    Note

    Funding agencies: Swedish Research Council (VR) [2013-5580]; Swedish Governmental Agency for Innovation Systems (VINNOVA) under the VINNMER international qualification program [2011-03486, 2014-04712]; Swedish foundation for strategic research (SSF) [FFL12-0181, RIF14-055]

    Available from: 2016-11-09 Created: 2016-11-09 Last updated: 2019-03-05Bibliographically approved
  • 31.
    Brodin, Håkan
    et al.
    Linköping University, Department of Management and Engineering, Engineering Materials. Linköping University, The Institute of Technology. Siemens Industrial Turbomachinery AB, Finspång, Sweden.
    Eriksson, Robert
    Siemens Industrial Turbomachinery AB, Finspång, Sweden.
    Johansson, Sten
    Siemens Industrial Turbomachinery AB, Finspång, Sweden.
    Sjöström, Sören
    Linköping University, Department of Management and Engineering, Solid Mechanics. Linköping University, The Institute of Technology. Siemens Industrial Turbomachinery AB, Finspång, Sweden.
    Fracture Mechanical Modelling of a Plasma Sprayed TBC System2009In: Advanced Ceramic Coatings and Interfaces IV / [ed] Dongming Zhu and Hua-Tay Lin, Westerville, OH, United States: American Ceramic Society Inc. , 2009, Vol. 30, no 3, p. 113-124Conference paper (Refereed)
    Abstract [en]

    A thermal barrier coating (TBC) system subjected to thermal cycling will develop a microcrack partem near the interface between the metallic bond coat and the ceramic top coat. These small cracks link up and form internal TBC delaminations during repeated heating / cooling. After a longer time period, the internal delamination cracks will form a larger spallation damage, where the TBC is detached from the underlying material. Since cracks are initiated in multiple sites of the thermal barrier coating, the damage is initially considered to be governed by local stress conditions. The purpose of the present work is to compare experimental data with predictions of a physically based fatigue life model. The present study has been performed on plasma-sprayed TBCs where the interface geometry has been varied. In the present work, calculation of fatigue life is done for a number of cases under thermal fatigue loading. Different interface geometries are compared in order to understand the influence of variations in the TC/BC interface roughness on oxidation behaviour and thermal fatigue life. Thermal fatigue tests indicate that an increased surface roughness is beneficial from a fatigue life point of view.

  • 32.
    Brooke, Robert
    et al.
    Linköping University, Department of Science and Technology. Linköping University, Faculty of Science & Engineering.
    Franco Gonzalez, Felipe
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Wijeratne, Kosala
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Pavlopoulou, Eleni
    Univ Bordeaux, France.
    Galliani, Daniela
    Univ Milano Bicocca, Italy.
    Liu, Xianjie
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Valiollahi Bisheh, Roudabeh
    Linköping University, Department of Science and Technology. Linköping University, Faculty of Science & Engineering.
    Zozoulenko, Igor
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Vapor phase synthesized poly(3,4-ethylenedioxy-thiophene)-trifluoromethanesulfonate as a transparent conductor material2018In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 6, no 43, p. 21304-21312Article in journal (Refereed)
    Abstract [en]

    Inorganic transparent conductive oxides have dominated the market as transparent electrodes due to their high conductivity and transparency. Here, we report the fabrication and optimization of the synthesis of poly(3,4-ethylenedioxythiophene) trifluoromethanesulfonate via vapor phase polymerization for the potential replacement of such inorganic materials. The parameters and conditions of the polymerization were investigated and an electrical conductivity of 3800 S cm(-1) and 4500 S cm(-1) after acid treatment were obtained while maintaining an absorbance similar to that of commercial indium tin oxide. This increase in electrical conductivity was rationalized experimentally and theoretically to an increase in the oxidation level and a higher order of crystallinity which does not disrupt the pi-pi stacking of PEDOT chains.

  • 33.
    Byeon, Ayeong
    et al.
    Drexel University, PA 19104 USA; Drexel University, PA 19104 USA; Korea Adv Institute Science and Technology, South Korea.
    Zhao, Meng-Qiang
    Drexel University, PA 19104 USA; Drexel University, PA 19104 USA.
    Ren, Chang E.
    Drexel University, PA 19104 USA; Drexel University, PA 19104 USA.
    Halim, Joseph
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering. Drexel University, PA 19104 USA; Drexel University, PA 19104 USA.
    Kota, Sankalp
    Drexel University, PA 19104 USA.
    Urbankowski, Patrick
    Drexel University, PA 19104 USA.
    Anasori, Babak
    Drexel University, PA 19104 USA.
    Barsoum, Michel W.
    Drexel University, PA 19104 USA.
    Gogotsi, Yury
    Drexel University, PA 19104 USA.
    Two-Dimensional Titanium Carbide MXene As a Cathode Material for Hybrid Magnesium/Lithium-Ion Batteries2017In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 9, no 5, p. 4296-4300Article in journal (Refereed)
    Abstract [en]

    As an alternative to pure lithium-ion, Lit, systems, a hybrid magnesium, Mg2+, and Li+ battery can potentially combine the high capacity, high voltage, and fast Li+ intercalation of Li-ion battery cathodes and the high capacity, low cost, and dendrite-free Mg metal anodes. Herein, we report on the use of two-dimensional titanium carbide, Ti3C2Tx (MXene), as a cathode in hybrid Mg2+/Li+ batteries, coupled with a Mg metal anode. Free-standing and flexible Ti3C2Tx/carbon nanotube composite "paper" delivered-,100 mAh at 0.1 C and similar to 50 mAh g(-1) at 10 C. At 1 C the capacity was maintained for amp;gt;500 cycles at 80 mAh g(-1). The Mo2CTx MXene also demonstrated good performance as a cathode material in this hybrid battery. Considering the variety of available MXenes, this work opens the door for exploring a new large family of 2D materials with high electrical conductivity and large intercalation capacity as cathodes for hybrid Mg2+/Li+ batteries.

  • 34.
    Bykov, M.
    et al.
    Univ Bayreuth, Germany.
    Bykova, E.
    Univ Bayreuth, Germany; DESY, Germany.
    Aprilis, G.
    Univ Bayreuth, Germany.
    Glazyrin, K.
    DESY, Germany.
    Koemets, E.
    Univ Bayreuth, Germany.
    Chuvashova, I
    Univ Bayreuth, Germany; Univ Bayreuth, Germany.
    Kupenko, I
    Univ Munster, Germany.
    McCammon, C.
    Univ Bayreuth, Germany.
    Mezouar, M.
    European Synchrotron Radiat Facil, France.
    Prakapenka, V
    Univ Chicago, IL 60437 USA.
    Liermann, H-P
    DESY, Germany.
    Tasnadi, Ferenc
    Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics. Linköping University, Faculty of Science & Engineering. Natl Univ Sci and Technol MISIS, Russia.
    Ponomareva, A. V
    Natl Univ Sci and Technol MISIS, Russia.
    Abrikosov, Igor
    Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics. Linköping University, Faculty of Science & Engineering.
    Dubrovinskaia, N.
    Univ Bayreuth, Germany.
    Dubrovinsky, L.
    Univ Bayreuth, Germany.
    Fe-N system at high pressure reveals a compound featuring polymeric nitrogen chains2018In: Nature Communications, ISSN 2041-1723, E-ISSN 2041-1723, Vol. 9, article id 2756Article in journal (Refereed)
    Abstract [en]

    Poly-nitrogen compounds have been considered as potential high energy density materials for a long time due to the large number of energetic N-N or N=N bonds. In most cases high nitrogen content and stability at ambient conditions are mutually exclusive, thereby making the synthesis of such materials challenging. One way to stabilize such compounds is the application of high pressure. Here, through a direct reaction between Fe and N-2 in a laser-heated diamond anvil cell, we synthesize three ironnitrogen compounds Fe3N2, FeN2 and FeN4. Their crystal structures are revealed by single-crystal synchrotron X-ray diffraction. Fe3N2, synthesized at 50 GPa, is isostructural to chromium carbide Cr3C2. FeN2 has a marcasite structure type and features covalently bonded dinitrogen units in its crystal structure. FeN4, synthesized at 106 GPa, features polymeric nitrogen chains of [N-4(2-)](n) units. Based on results of structural studies and theoretical analysis, [N-4(2-)](n) units in this compound reveal catena-poly[tetraz-1-ene-1,4-diyl] anions.

  • 35.
    Bykova, E.
    et al.
    DESY, Germany; Univ Bayreuth, Germany.
    Bykov, M.
    Univ Bayreuth, Germany; Natl Univ Sci and Technol MISIS, Russia.
    Cernok, A.
    Univ Bayreuth, Germany; Open Univ, England.
    Tidholm, Johan
    Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics. Linköping University, Faculty of Science & Engineering.
    Simak, Sergey
    Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics. Linköping University, Faculty of Science & Engineering.
    Hellman, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics. Linköping University, Faculty of Science & Engineering. CALTECH, CA 91125 USA.
    Belov, M. P.
    Natl Univ Sci and Technol MISIS, Russia.
    Abrikosov, Igor
    Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics. Linköping University, Faculty of Science & Engineering.
    Liermann, H. -P.
    DESY, Germany.
    Hanfland, M.
    European Synchrotron Radiat Facil, France.
    Prakapenka, V. B.
    Univ Chicago, IL 60637 USA.
    Prescher, C.
    Univ Chicago, IL 60637 USA; Univ Cologne, Germany.
    Dubrovinskaia, N.
    Univ Bayreuth, Germany.
    Dubrovinsky, L.
    Univ Bayreuth, Germany.
    Metastable silica high pressure polymorphs as structural proxies of deep Earth silicate melts2018In: Nature Communications, ISSN 2041-1723, E-ISSN 2041-1723, Vol. 9, article id 4789Article in journal (Refereed)
    Abstract [en]

    Modelling of processes involving deep Earth liquids requires information on their structures and compression mechanisms. However, knowledge of the local structures of silicates and silica (SiO2) melts at deep mantle conditions and of their densification mechanisms is still limited. Here we report the synthesis and characterization of metastable high-pressure silica phases, coesite-IV and coesite-V, using in situ single-crystal X-ray diffraction and ab initio simulations. Their crystal structures are drastically different from any previously considered models, but explain well features of pair-distribution functions of highly densified silica glass and molten basalt at high pressure. Built of four, five-, and six-coordinated silicon, coesite-IV and coesite-V contain SiO6 octahedra, which, at odds with 3rd Paulings rule, are connected through common faces. Our results suggest that possible silicate liquids in Earths lower mantle may have complex structures making them more compressible than previously supposed.

  • 36.
    Börjesson, Anders
    et al.
    Högskolan i Borås, Institutionen Ingenjörshögskolan.
    Erdtman, Edvin
    Högskolan i Borås, Institutionen Ingenjörshögskolan.
    Ahlström, Peter
    Högskolan i Borås, Institutionen Ingenjörshögskolan.
    Berlin, Mikael
    Tetra Pak Packaging Solutions AB, Ruben Rausings gata, Lund, Sweden.
    Andersson, Thorbjörn
    Tetra Pak Packaging Solutions AB, Ruben Rausings gata, Lund, Sweden.
    Bolton, Kim
    Högskolan i Borås, Institutionen Ingenjörshögskolan.
    Molecular modelling of oxygen and water permeation in polyethylene2013In: Polymer, ISSN 0032-3861, E-ISSN 1873-2291, Vol. 54, no 12, p. 2988-Article in journal (Refereed)
    Abstract [en]

    Monte Carlo and molecular dynamics simulations were performed to calculate solubility, S, and diffusion, D, coefficients of oxygen and water in polyethylene, and to obtain a molecular-level understanding of the diffusion mechanism. The permeation coefficient, P, was calculated from the product of S and D. The AMBER force field, which yields the correct polymer densities under the conditions studied, was used for the simulations, and it was observed that the results were not sensitive to the inclusion of atomic charges in the force field. The simulated S for oxygen and water are higher and lower than experimental data, respectively. The calculated diffusion coefficients are in good agreement with experimental data. Possible reasons for the discrepancy in the simulated and experimental solubilities, which results in discrepancies in the permeation coefficients, are discussed. The diffusion of both penetrants occurs mainly by large amplitude, infrequent jumps of the molecules through the polymer matrix.

  • 37.
    Cai, Liangliang
    et al.
    Tongji Univ, Peoples R China.
    Yu, Xin
    Tongji Univ, Peoples R China.
    Liu, Mengxi
    Natl Ctr Nanosci and Technol, Peoples R China.
    Sun, Qiang
    Tongji Univ, Peoples R China.
    Bao, Meiling
    Tongji Univ, Peoples R China.
    Zha, Zeqi
    Natl Ctr Nanosci and Technol, Peoples R China; Univ Chinese Acad Sci, Peoples R China.
    Pan, Jinliang
    Natl Ctr Nanosci and Technol, Peoples R China; Univ Chinese Acad Sci, Peoples R China.
    Ma, Honghong
    Tongji Univ, Peoples R China.
    Ju, Huanxin
    Univ Sci and Technol China, Peoples R China.
    Hu, Shanwei
    Univ Sci and Technol China, Peoples R China.
    Xu, Liang
    Tongji Univ, Peoples R China.
    Zou, Jiacheng
    Tongji Univ, Peoples R China.
    Yuan, Chunxue
    Tongji Univ, Peoples R China.
    Jacob, Timo
    Ulm Univ, Germany.
    Björk, Jonas
    Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics. Linköping University, Faculty of Science & Engineering.
    Zhu, Junfa
    Univ Sci and Technol China, Peoples R China.
    Qu, Xiaohui
    Natl Ctr Nanosci and Technol, Peoples R China; Univ Chinese Acad Sci, Peoples R China.
    Xu, Wei
    Tongji Univ, Peoples R China.
    Direct Formation of C-C Double-Bonded Structural Motifs by On-Surface Dehalogenative Homocoupling of gem-Dibromomethyl Molecules2018In: ACS Nano, ISSN 1936-0851, E-ISSN 1936-086X, Vol. 12, no 8, p. 7959-7966Article in journal (Refereed)
    Abstract [en]

    Conductive polymers are of great importance in a variety of chemistry-related disciplines and applications. The recently developed bottom-up on-surface synthesis strategy provides us with opportunities for the fabrication of various nanostructures in a flexible and facile manner, which could be investigated by high-resolution microscopic techniques in real space. Herein, we designed and synthesized molecular precursors functionalized with benzal gem-dibromomethyl groups. A combination of scanning tunneling microscopy, noncontact atomic force microscopy, high-resolution synchrotron radiation photoemission spectroscopy, and density functional theory calculations demonstrated that it is feasible to achieve the direct formation of C-C double-bonded structural motifs via on-surface dehalogenative homocoupling reactions on the Au(111) surface. Correspondingly, we convert the sp(3)-hybridized state to an sp(2)-hybridized state of carbon atoms, i.e., from an alkyl group to an alkenyl one. Moreover, by such a bottom-up strategy, we have successfully fabricated poly(phenylenevinylene) chains on the surface, which is anticipated to inspire further studies toward understanding the nature of conductive polymers at the atomic scale.

  • 38.
    Carlsson, Andreas
    Linköping University, Department of Physics, Chemistry and Biology, Chemistry. Linköping University, Faculty of Science & Engineering. Swedish National Forens Centre NFC, Linkoping, Sweden.
    Synthesis and spectroscopic characterization of emerging synthetic cannabinoids and cathinones2016Licentiate thesis, comprehensive summary (Other academic)
    Abstract [en]

    The application of different analytical techniques is fundamental in forensic drug analysis. In the wake of the occurrence of large numbers of new psychoactive substances possessing similar chemical structures as already known ones, focus has been placed on applied criteria for their univocal identification. These criteria vary, obviously, depending on the applied technique and analytical approach. However, when two or more substances are proven to have similar analytical properties, these criteria no longer apply, which imply that complementary techniques have to be used in their differentiation.

    This work describes the synthesis of some structural analogues to synthetic cannabinoids and cathinones based on the evolving patterns in the illicit drug market. Six synthetic cannabinoids and six synthetic cathinones were synthesized, that, at the time for this study, were not as yet found in drug seizures. Further, a selection of their spectroscopic data is compared to those of already existing analogues; mainly isomers and homologues. The applied techniques were mass spectrometry (MS), Fourier transformed infrared (FTIR, gas phase) spectroscopy and nuclear magnetic resonance (NMR) spectroscopy. In total, 59 different compounds were analyzed with the  selected techniques.

    The results from comparison of spectroscopic data showed that isomeric substances may in some cases be difficult to unambiguously identify based only on their GC-MS EI spectra. On the other hand, GC-FTIR demonstrated more distinguishable spectra. The spectra for the homologous compounds showed however, that the GC-FTIR technique was less successful compared to GC-MS. Also a pronounced fragmentation pattern for some of the cathinones was found.

    In conclusion, this thesis highlights the importance of using complementary techniques for the univocal identification of synthetic cannabinoids and cathinones. By increasing the number of analogues investigated, the more may be learnt about the capabilities of different techniques for structural differentiations, and thereby providing important identification criteria leading to trustworthy forensic evidence.

    List of papers
    1. Prediction of designer drugs: synthesis and spectroscopic analysis of synthetic cannabinoid analogues of 1H-indol-3-yl(2,2,3,3-tetramethylcyclopropyl) methanone and 1H-indol-3-yl(adamantan-1-yl)methanone
    Open this publication in new window or tab >>Prediction of designer drugs: synthesis and spectroscopic analysis of synthetic cannabinoid analogues of 1H-indol-3-yl(2,2,3,3-tetramethylcyclopropyl) methanone and 1H-indol-3-yl(adamantan-1-yl)methanone
    Show others...
    2016 (English)In: Drug Testing and Analysis, ISSN 1942-7603, E-ISSN 1942-7611, Vol. 8, no 10, p. 1015-1029Article in journal (Refereed) Published
    Abstract [en]

    In this work, emergence patterns of synthetic cannabinoids were utilized in an attempt to predict those that may appear on the drug market in the future. Based on this information, two base structures of the synthetic cannabinoid analogues - (1H-indol-3-yl (2,2,3,3-tetramethylcyclopropyl) methanone and 1H-indol-3-yl(adamantan-1-yl)methanone) - together with three substituents butyl, 4-fluorobutyl and ethyl tetrahydropyran - were selected for synthesis. This resulted in a total of six synthetic cannabinoid analogues that to the authors knowledge have not yet appeared on the drug market. Spectroscopic data, including nuclearmagnetic resonance (NMR), mass spectrometry (MS), and Fourier transforminfrared (FTIR) spectroscopy (solid and gas phase), are presented for the synthesized analogues and some additional related cannabinoids. In this context, the suitability of the employed techniques for the identification of unknowns is discussed and the use of GC-FTIR as a secondary complementary technique to GC-MS is addressed. Examples of compounds that are difficult to differentiate by their mass spectra, but can be distinguished based upon their gas phase FTIR spectra are presented. Conversely, structural homologueswhere mass spectra aremore powerful than gas phase FTIR spectra for unambiguous assignments are also exemplified. This work further emphasizes that a combination of several techniques is the key to success in structural elucidations. Copyright (C) 2015 John Wiley amp; Sons, Ltd.

    Place, publisher, year, edition, pages
    WILEY-BLACKWELL, 2016
    Keywords
    drug analysis; proactive; synthetic cannabinoids; synthesis; mass spectrometry
    National Category
    Pharmaceutical Sciences
    Identifiers
    urn:nbn:se:liu:diva-132473 (URN)10.1002/dta.1904 (DOI)000384806400003 ()26526273 (PubMedID)
    Note

    Funding Agencies|Swedish Contingencies Agency (MSB)

    Available from: 2016-11-13 Created: 2016-11-12 Last updated: 2018-01-13
  • 39.
    Cattelan, Mattia
    et al.
    School of Chemistry, University of Bristol, Cantocks Close, Bristol, United Kingdom.
    Vagin, Mikhail
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Fox, Neil A.
    School of Chemistry, University of Bristol, Cantocks Close, Bristol, United Kingdom.
    Ivanov, Ivan Gueorguiev
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Shtepliuk, Ivan
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Anodization study of epitaxial graphene: insights on the oxygen evolution reaction of graphitic materials2019In: Nanotechnology, ISSN 0957-4484, E-ISSN 1361-6528, Vol. 30, no 28, article id 285701Article in journal (Refereed)
    Abstract [en]

    The photoemission electron microscopy and x-ray photoemission spectroscopy were utilized for the study of anodized epitaxial graphene (EG) on silicon carbide as a fundamental aspect of the oxygen evolution reaction on graphitic materials. The high-resolution analysis of surface morphology and composition quantified the material transformation during the anodization. We investigated the surface with lateral resolution amp;lt;150 nm, revealing significant transformations on the EG and the role of multilayer edges in increasing the film capacitance.

  • 40.
    Chalangar, Ebrahim
    Linköping University, Department of Science and Technology, Physics, Electronics and Mathematics. Linköping University, Faculty of Science & Engineering.
    Graphene-based nanocomposites for electronics and photocatalysis2019Licentiate thesis, comprehensive summary (Other academic)
    Abstract [en]

    The development of future electronics depends on the availability of suitable functional materials. Printed electronics, for example, relies on access to highly conductive, inexpensive and printable materials, while strong light absorption and low carrier recombination rates are demanded in photocatalysis industry. Despite all efforts to develop new materials, it still remains a challenge to have all the desirable aspects in a single material. One possible route towards novel functional materials, with improved and unprecedented physical properties, is to form composites of different selected materials.

    In this work, we report on hydrothermal growth and characterization of graphene/zinc oxide (GR/ZnO) nanocomposites, suited for electronics and photocatalysis application. For conductive purposes, highly Al-doped ZnO nanorods grown on graphene nanoplates (GNPs) prevent the GNPs from agglomerating and promote conductive paths between the GNPs. The effect of the ZnO nanorod morphology and GR dispersity on the nanocomposite conductivity and GR/ZnO nanorod bonding strength were investigated by conductivity measurements and optical spectroscopy. The inspected samples show that growth in high pH solutions promotes a better graphene dispersity, higher doping and enhanced bonding between the GNPs and the ZnO nanorods. Growth in low pH solutions yield samples characterized by a higher conductivity and a reduced number of surface defects.

    In addition, different GR/ZnO nanocomposites, decorated with plasmonic silver iodide (AgI) nanoparticles, were synthesized and analyzed for solar-driven photocatalysis. The addition of Ag/AgI generates a strong surface plasmon resonance effect involving metallic Ag0, which redshifts the optical absorption maximum into the visible light region enhancing the photocatalytic performance under solar irradiation. A wide range of characterization techniques including, electron microscopy, photoelectron spectroscopy and x-ray diffraction confirm a successful formation of photocatalysts.

    Our findings show that the novel proposed GR-based nanocomposites can lead to further development of efficient photocatalyst materials with applications in removal of organic pollutants, or for fabrication of large volumes of inexpensive porous conjugated GR-semiconductor composites.

    List of papers
    1. Influence of morphology on electrical and optical properties of graphene/Al-doped ZnO-nanorod composites
    Open this publication in new window or tab >>Influence of morphology on electrical and optical properties of graphene/Al-doped ZnO-nanorod composites
    Show others...
    2018 (English)In: Nanotechnology, ISSN 0957-4484, E-ISSN 1361-6528, Vol. 29, no 41, article id 415201Article in journal (Refereed) Published
    Abstract [en]

    The development of future 3D-printed electronics relies on the access to highly conductive inexpensive materials that are printable at low temperatures (amp;lt;100 degrees C). The implementation of available materials for these applications are, however, still limited by issues related to cost and printing quality. Here, we report on the simple hydrothermal growth of novel nanocomposites that are well suited for conductive printing applications. The nanocomposites comprise highly Al-doped ZnO nanorods grown on graphene nanoplatelets (GNPs). The ZnO nanorods play the two major roles of (i) preventing GNPs from agglomerating and (ii) promoting electrical conduction paths between the graphene platelets. The effect of two different ZnO-nanorod morphologies with varying Al-doping concentration on the nanocomposite conductivity and the graphene dispersity are investigated. Time-dependent absorption, photoluminescence and photoconductivity measurements show that growth in high pH solutions promotes a better graphene dispersity, higher doping levels and enhanced bonding between the graphene and the ZnO nanorods. Growth in low pH solutions yields samples characterized by a higher conductivity and a reduced number of surface defects. These samples also exhibit a large persistent photoconductivity attributed to an effective charge separation and transfer from the nanorods to the graphene platelets. Our findings can be used to tailor the conductivity of novel printable composites, or for fabrication of large volumes of inexpensive porous conjugated graphene-semiconductor composites.

    Place, publisher, year, edition, pages
    Institute of Physics Publishing (IOPP), 2018
    Keywords
    graphene; zinc oxide; nanorods; nanocomposites; persistent photoconductivity; printing
    National Category
    Materials Chemistry
    Identifiers
    urn:nbn:se:liu:diva-150196 (URN)10.1088/1361-6528/aad3ec (DOI)000440632800001 ()30015332 (PubMedID)2-s2.0-85051665865 (Scopus ID)
    Note

    Funding Agencies|Knowledge Foundation; Linkoping University; Halmstad University

    Available from: 2018-08-22 Created: 2018-08-22 Last updated: 2019-05-28Bibliographically approved
  • 41.
    Chalangar, Ebrahim
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering. Halmstad Univ, Sweden.
    Machhadani, Houssaine
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Lim, Seung-Hyuk
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Karlsson, Fredrik
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Nur, Omer
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Willander, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Pettersson, Håkan
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering. Halmstad Univ, Sweden; Lund Univ, Sweden; Lund Univ, Sweden.
    Influence of morphology on electrical and optical properties of graphene/Al-doped ZnO-nanorod composites2018In: Nanotechnology, ISSN 0957-4484, E-ISSN 1361-6528, Vol. 29, no 41, article id 415201Article in journal (Refereed)
    Abstract [en]

    The development of future 3D-printed electronics relies on the access to highly conductive inexpensive materials that are printable at low temperatures (amp;lt;100 degrees C). The implementation of available materials for these applications are, however, still limited by issues related to cost and printing quality. Here, we report on the simple hydrothermal growth of novel nanocomposites that are well suited for conductive printing applications. The nanocomposites comprise highly Al-doped ZnO nanorods grown on graphene nanoplatelets (GNPs). The ZnO nanorods play the two major roles of (i) preventing GNPs from agglomerating and (ii) promoting electrical conduction paths between the graphene platelets. The effect of two different ZnO-nanorod morphologies with varying Al-doping concentration on the nanocomposite conductivity and the graphene dispersity are investigated. Time-dependent absorption, photoluminescence and photoconductivity measurements show that growth in high pH solutions promotes a better graphene dispersity, higher doping levels and enhanced bonding between the graphene and the ZnO nanorods. Growth in low pH solutions yields samples characterized by a higher conductivity and a reduced number of surface defects. These samples also exhibit a large persistent photoconductivity attributed to an effective charge separation and transfer from the nanorods to the graphene platelets. Our findings can be used to tailor the conductivity of novel printable composites, or for fabrication of large volumes of inexpensive porous conjugated graphene-semiconductor composites.

  • 42.
    Charrier, Dimitri S. H.
    et al.
    Eindhoven University of Technology, Netherlands.
    Janssen, Rene A. J.
    Eindhoven University of Technology, Netherlands.
    Kemerink, Martijn
    Eindhoven University of Technology, Netherlands.
    Large Electrically Induced Height and Volume Changes in Poly(3,4-ethylenedioxythiophene)/Poly(styrenesulfonate) Thin Films2010In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 22, no 12, p. 3670-3677Article in journal (Refereed)
    Abstract [en]

    We demonstrate large, partly reversible height and volume changes of thin films of poly(3,4-ethylenedioxythiophene)/poly(styrenesulfonate) (PEDOT:PSS) on the anode of interdigitating gold electrodes under ambient conditions by applying an electrical bias. The height and volume changes were monitored with optical and atomic force microscopy and are found to be independent of initial film thickness. In the first cycle, a relative height change of 950% is observed for a 21 nm thick film. Two regimes are identified. In the first regime, reversible redox reactions occur and reversible height changes can be ascribed to absorption of water via osmotic effects, brought about by an increasing ion concentration on the anode. In the second, irreversible regime, irreversible overoxidation of the PEDOT occurs and mass transport from the channel to the anode becomes important.

  • 43.
    Chen, Youchun
    et al.
    Jilin University, Peoples R China.
    Wang, Shan
    Jilin University, Peoples R China.
    Xue, Lingwei
    Chinese Academic Science, Peoples R China.
    Zhang, Zhiguo
    Chinese Academic Science, Peoples R China.
    Li, Haolong
    Jilin University, Peoples R China.
    Wu, Lixin
    Jilin University, Peoples R China.
    Wang, Yue
    Jilin University, Peoples R China.
    Li, Fenghong
    Jilin University, Peoples R China.
    Zhang, Fengling
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Li, Yongfang
    Chinese Academic Science, Peoples R China.
    Insights into the working mechanism of cathode interlayers in polymer solar cells via [(C8H17)(4)N](4)[SiW12O40]2016In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 4, no 48, p. 19189-19196Article in journal (Refereed)
    Abstract [en]

    A low-cost (amp;lt;$1 per g), high-yield (amp;gt;90%), alcohol soluble surfactant-encapsulated polyoxometalate complex [(C8H17)(4)N](4)[SiW12O40] has been synthesized and utilized as a cathode interlayer (CIL) in polymer solar cells (PSCs). A power conversion efficiency of 10.1% can be obtained for PSCs based on PTB7-Th (poly[[2,6-4,8-di(5-ethylhexylthienyl) benzo[1,2-b;3,3-b]-dithiophene][3-fluoro-2[(2-ethylhexyl) carbonyl] thieno [3,4-b]-thiophenediyl]]):PC71BM ([6,6]-phenyl C71-butyric acidmethyl ester) due to the incorporation of [(C8H17)(4)N](4)[SiW12O40]. Combined measurements of current density-voltage characteristics, transient photocurrent, charge carrier mobility and capacitance-voltage characteristics demonstrate that [(C8H17)(4)N](4)[SiW12O40] can effectively increase the built-in potential, charge carrier density and mobility and accelerate the charge carrier extraction in PSCs. Most importantly, the mechanism of using [(C8H17)(4)N](4)[SiW12O40] as the CIL is further brought to light by X-ray photoemission spectroscopy (XPS) and ultraviolet photoemission spectroscopy (UPS) of the metal/ [(C8H17)(4)N](4)[SiW12O40] interface. The findings suggest that [(C8H17)(4)N](4)[SiW12O40] not only decreased the work function of the metal cathodes but also was n-doped upon contact with the metals, which provide insights into the working mechanism of the CILs simultaneously improving the open circuit voltage, short circuit current and fill factor in the PSCs.

  • 44.
    Chen, Zhe
    et al.
    Linköping University, Department of Management and Engineering, Engineering Materials. Linköping University, Faculty of Science & Engineering.
    Hörnqvist Colliander, Magnus
    Department of Physics, Chalmers University of Technology, Gothenburg, Sweden.
    Sundell, Gustav
    Department of Physics, Chalmers University of Technology, Gothenburg, Sweden.
    Peng, Ru
    Linköping University, Department of Management and Engineering, Engineering Materials. Linköping University, Faculty of Science & Engineering.
    Zhou, Jinming
    Division of Production and Materials Engineering, Lund University, Sweden.
    Johansson, Sten
    Linköping University, Department of Management and Engineering, Engineering Materials. Linköping University, Faculty of Science & Engineering.
    Moverare, Johan
    Linköping University, Department of Management and Engineering, Engineering Materials. Linköping University, Faculty of Science & Engineering.
    Nano-scale characterization of white layer in broached Inconel 7182017In: Materials Science & Engineering: A, ISSN 0921-5093, E-ISSN 1873-4936, Vol. 684, p. 373-384Article in journal (Refereed)
    Abstract [sv]

    The formation mechanism of white layers during broaching and their mechanical properties are not well investigated and understood to date. In the present study, multiple advanced characterization techniques with nano-scale resolution, including transmission electron microscopy (TEM), transmission Kikuchi diffraction (TKD), atom probe tomography (APT) as well as nano-indentation, have been used to systematically examine the microstructural evolution and corresponding mechanical properties of a surface white layer formed when broaching the nickel-based superalloy Inconel 718.

    TEM observations showed that the broached white layer consists of nano-sized grains, mostly in the range of 20–50 nm. The crystallographic texture detected by TKD further revealed that the refined microstructure is primarily caused by strong shear deformation. Co-located Al-rich and Nb-rich fine clusters have been identified by APT, which are most likely to be γ′ and γ′′ clusters in a form of co-precipitates, where the clusters showed elongated and aligned appearance associated with the severe shearing history. The microstructural characteristics and crystallography of the broached white layer suggest that it was essentially formed by adiabatic shear localization in which the dominant metallurgical process is rotational dynamic recrystallization based on mechanically-driven subgrain rotations. The grain refinement within the white layer led to an increase of the surface nano-hardness by 14% and a reduction in elastic modulus by nearly 10% compared to that of the bulk material. This is primarily due to the greatly increased volume fraction of grain boundaries, when the grain size was reduced down to the nanoscale.

  • 45.
    Conings, Bert
    et al.
    Hasselt University, Belgium; University of Oxford, England.
    Babayigit, Aslihan
    Hasselt University, Belgium; University of Oxford, England.
    Klug, Matthew T.
    University of Oxford, England.
    Bai, Sai
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering. University of Oxford, England.
    Gauquelin, Nicolas
    University of Antwerp, Belgium.
    Sakai, Nobuya
    University of Oxford, England.
    Tse-Wei Wang, Jacob
    University of Oxford, England.
    Verbeeck, Johan
    University of Antwerp, Belgium.
    Boyen, Hans-Gerd
    Hasselt University, Belgium.
    Snaith, Henry J.
    University of Oxford, England.
    A Universal Deposition Protocol for Planar Heterojunction Solar Cells with High Efficiency Based on Hybrid Lead Halide Perovskite Families2016In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 28, no 48, p. 10701-+Article in journal (Refereed)
    Abstract [en]

    A robust and expedient gas quenching method is developed for the solution deposition of hybrid perovskite thin films. The method offers a reliable standard practice for the fabrication of a non-exhaustive variety of perovskites exhibiting excellent film morphology and commensurate high performance in both regular and inverted structured solar cell architectures.

  • 46.
    Danielsson, Örjan
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
    Simulations of Silicon Carbide Chemical Vapor Deposition2002Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Most of the modern electronics technology is based on the semiconducting material silicon. The increasing demands for smaller electronic devices with improved performance at lower costs drive the conventional silicon technology to its limits. To meet the requirements from the industry and to explore new application areas, other materials and fabrication methods must be used. For devices operating at high powers, high temperatures and high frequencies, the so-called wide bandgap semiconductors can be used with great success. Silicon carbide (SiC) and III-nitrides are wide bandgap materials that have gained increased interest in recent years. One important technique in manufacturing of electronic devices is chemical vapor deposition (CVD), by which thin layers can be deposited. These layers may have different electrical properties, depending on the choice of material and doping. Generally in CVD, a reactive gas mixture flows through a heated reactor chamber, where the substrates are placed. Complex chemical reactions take place in the gas and on the substrate surface, leading to many intermediate species and by-products, and eventually to the desired deposition. For the growth of device quality material it is important to be able to control the properties of the grown layers. These properties generally depend on the growth conditions in the reaction chamber, and on the chemistry of the deposition process. So far, empirical trial-and-error methods have been employed in the development of growth processes. Due to the lack of basic understanding of the governing physical processes, progress is costly and time consuming. Improving and optimizing the CVD process, as well as improving the fundamental understanding of the whole process is of great importance when good quality material should be produced. For this, computer simulations of the relevant physical and chemical phenomena can provide the necessary tools. This thesis focuses on computer simulations of the CVD process, in particular CVD of SiC. Simulations can be used not only as a tool for optimizing growth processes and reactor designs, they can also give information about physical phenomena that are difficult to measure, such as the gas-phase composition or the flow paths inside the reactor.

    Heating of the CVD susceptor is a central part of the process. For the growth of high quality SiC a relatively high temperature must be used. A convenient method for heating to high temperatures is by induction. A low resistive material, such as graphite, is placed inside a coil, which is given an alternating current. The graphite is then heated by the induced currents due to ohmic resistance. In this thesis the temperature distribution inside a CVD reactor, and how it is influenced by changes in coil frequency, power input to the coil and graphite thickness, is investigated. It is shown that by changing the placement and shape of the coil and by using insulation material correctly, a more uniform temperature distribution can be obtained.

    A model for the growth of SiC is used to predict growth rates at various process parameters. A number of possible factors influencing the growth rate are investigated using this model. The importance of including thermal diffusion and the effect of etching by hydrogen is shown, and the effect of parasitic growth investigated. Simulations show a mass transport limited growth, as seen from experiments.

    An improved susceptor design with an up-lifted substrate holder plate is investigated and compared to a conventional hot-wall reactor and to a cold-wall reactor. It is shown that stress induced by thermal gradients through the substrate is significantly reduced in the hot-wall reactor, and that stress due to backside growth can be diminished using the new design. Positive side effects are that slightly higher growth rates can be achieved, and that the growth temperature can be slightly lowered in the new susceptor.

    The doping incorporation behavior is thoroughly investigated experimentally for intentional doping with nitrogen and aluminum. The doping incorporation on both faces of SiC, as well as on two different polytypes is investigated. Equilibrium calculations are preformed, giving possible candidates for species responsible for the doping incorporation. To predict nitrogen doping concentrations, a simplified quantitative model is developed and applied to a large number of process parameters. It is seen that the same species as predicted by equilibrium calculations are produced, but the reactions producing these species are relatively slow, so that the highest concentrations are at the outlet of the reactor. It is thus concluded that N2 must be the major specie responsible for the nitrogen incorporation in SiC.

    For the growth of III-nitrides, ammonia is often used to give the nitrogen needed. It is well known that ammonia forms a solid adduct with the metalorganic gas, which is used as the source for the group III elements. It would thus be beneficial to use some other gas instead of ammonia. Since purity is of great importance, N2 gas would be the preferred choice. However, N2 is a very stable molecule and difficult to crack, even at high temperatures. It is shown that hydrogen can help in cracking nitrogen, and that growth of III-nitrides can be performed using N2 as the nitrogen-bearing gas, by only small changes to a conventional hot-wall CVD reactor.

    List of papers
    1. Investigation of the temperature profile in a hot-wall SiC chemical vapour deposition reactor
    Open this publication in new window or tab >>Investigation of the temperature profile in a hot-wall SiC chemical vapour deposition reactor
    2002 (English)In: Journal of Crystal Growth, ISSN 0022-0248, E-ISSN 1873-5002, Vol. 235, no 1-4, p. 352-364Article in journal (Refereed) Published
    Abstract [en]

    The chemical vapor deposition (CVD) technique is widely used to grow epitaxial layers of silicon carbide. To meet the demands for high quality epitaxial layers, which have good morphology and a minimum variation of the doping and thickness, a good knowledge of the CVD process is essential. The present work uses a simulation tool to investigate several parameters influencing the heating of <!--[if !vml]--><!--[endif]-->a hot-wall CVD reactor. The simulations are set up as 2D axisymmetric problems and validation is made in a 2D horizontal hot-wall CVD reactor. By applying the knowledge achieved from the simulations, the temperature profile is optimized to give as large area as possible with homogeneous temperature. New susceptor and coil designs are tested. A very good agreement between the simulated and the measured results is obtained. The new design has a temperature variation of less than 0.5% over more than 70% of the total susceptor length at an operating temperature of 1650°C. In addition, the power input needed to reach the operating temperature is decreased by 15% compared to the original design. 3D simulations are performed to show that the changes made in the 2D case give similar results for the real 3D case.

    Place, publisher, year, edition, pages
    ScienceDirect, 2002
    Keywords
    A1. Computer simulation, A1. Heat transfer, A3. Chemical, vapor deposition, A3. Hot-wall epitaxy, B2. Semiconducting silicon carbide
    National Category
    Other Engineering and Technologies not elsewhere specified
    Identifiers
    urn:nbn:se:liu:diva-15064 (URN)10.1016/S0022-0248(01)01831-0 (DOI)
    Available from: 2008-10-13 Created: 2008-10-13 Last updated: 2017-12-11Bibliographically approved
    2.
    The record could not be found. The reason may be that the record is no longer available or you may have typed in a wrong id in the address field.
    3. Predicted nitrogen doping concentrations in silicon carbide epitaxial layers grown by hot-wall chemical vapor deposition
    Open this publication in new window or tab >>Predicted nitrogen doping concentrations in silicon carbide epitaxial layers grown by hot-wall chemical vapor deposition
    2003 (English)In: Journal of Crystal Growth, ISSN 0022-0248, E-ISSN 1873-5002, Vol. 250, no 3-4, p. 471-478Article in journal (Refereed) Published
    Abstract [en]

    A simple quantitative model for the surface adsorption of nitrogen has been developed to simulate the doping incorporation in intentionally doped 4H-SiC samples during epitaxial growth. Different reaction schemes are necessary for the two faces of SiC. The differences are discussed, and implications to the necessary model adjustments are stressed. The simulations are validated by experimental values for a large number of different process parameters with good agreement.

    Keywords
    A1. Doping, A1. Growth models, A3. Chemical vapor deposition, A3. Hot wall epitaxy, B2. Semiconducting silicon carbide
    National Category
    Engineering and Technology
    Identifiers
    urn:nbn:se:liu:diva-46680 (URN)10.1016/S0022-0248(02)02513-7 (DOI)
    Available from: 2009-10-11 Created: 2009-10-11 Last updated: 2017-12-13
    4. Reducing stress in silicon carbide epitaxial layers
    Open this publication in new window or tab >>Reducing stress in silicon carbide epitaxial layers
    2003 (English)In: Journal of Crystal Growth, ISSN 0022-0248, E-ISSN 1873-5002, Vol. 252, no 1-3, p. 289-296Article in journal (Refereed) Published
    Abstract [en]

    A susceptor for the epitaxial growth of silicon carbide, with an up-lifted substrate holder, is investigated and compared to other susceptor designs both experimentally and by the use of computational fluid dynamics simulations. It is shown that the wafer bending due to temperature gradients is diminished in a hot-wall reactor compared to growth in a cold-wall reactor. The substrate backside growth is diminished using the up-lifted substrate holder, limiting the substrate bending due to the backside growth. Thereby the stress built into the epitaxial layers during growth is significantly reduced. Simulations indicate a lower effective C/Si ratio over the wafer, and a lower preferable growth temperature, as compared to the original susceptor design. In addition a slightly higher growth rate is achieved

    Place, publisher, year, edition, pages
    Elsevier, 2003
    Keywords
    A1. Computer simulation; A3. Chemical vapor deposition; A3. Hot wall epitaxy; B2. Semiconducting silicon carbide
    National Category
    Condensed Matter Physics Other Physics Topics
    Identifiers
    urn:nbn:se:liu:diva-104590 (URN)10.1016/S0022-0248(03)00938-2 (DOI)
    Available from: 2014-02-19 Created: 2014-02-19 Last updated: 2017-12-06Bibliographically approved
    5. Using N2 as precursor gas in III-nitride CVD growth
    Open this publication in new window or tab >>Using N2 as precursor gas in III-nitride CVD growth
    2003 (English)In: Journal of Crystal Growth, ISSN 0022-0248, E-ISSN 1873-5002, Vol. 253, no 1-4, p. 26-37Article in journal (Refereed) Published
    Abstract [en]

    Computational fluid dynamics simulations have been performed to explore the possibility of using nitrogen gas as a precursor to III-nitride growth. A chemical model for the gas-phase decomposition of N2 has been used to show that large enough amounts of reactive species can be formed under conditions not far from those used in normal metalorganic chemical vapor deposition. Simulations were performed in 2D for various concentrations of N2, and comparisons with the use of NH3 were made. A modified reactor design needed to achieve high enough concentrations of reactive species is suggested. The possibility to increase the growth rate and material quality in III-nitride growth is discussed.

    Place, publisher, year, edition, pages
    Elsevier, 2003
    Keywords
    A1. Computer simulation; A1. Growth models; A3. Hot wall epitaxy; A3. Metalorganic chemical vapor deposition; B2. Semiconducting III–V materials
    National Category
    Materials Chemistry
    Identifiers
    urn:nbn:se:liu:diva-104589 (URN)10.1016/S0022-0248(03)00971-0 (DOI)
    Available from: 2014-02-19 Created: 2014-02-19 Last updated: 2017-12-06Bibliographically approved
    6. Nitrogen doping of epitaxial Silicon Carbide
    Open this publication in new window or tab >>Nitrogen doping of epitaxial Silicon Carbide
    Show others...
    2002 (English)In: Journal of Crystal Growth, ISSN 0022-0248, E-ISSN 1873-5002, Vol. 236, no 1-3, p. 101-112Article in journal (Refereed) Published
    Abstract [en]

    Intentional doping with nitrogen of 4H- and 6H-SiC has been performed using a hot-wall CVD reactor. The nitrogen doping dependence on the temperature, pressure, C/Si ratio, growth rate and nitrogen flow has been investigated. The nitrogen incorporation for C-face material showed to be C/Si ratio independent, whereas the doping decreased with increasing C/Si ratio for the Si-face material in accordance with the “site-competition” model. The nitrogen incorporation was constant in a temperature “window” of 75°C on Si-face material indicating a mass transport limited incorporation. Increasing the growth rate resulted in a decrease of nitrogen incorporation on Si-face but an increase on C-face material. Finally, a comparison between previously published results on cold-wall CVD-grown material and the present hot-wall-grown material is presented.

    Place, publisher, year, edition, pages
    ScienceDirect, 2002
    Keywords
    A1. Doping, A3. Hot wall epitaxy, B2. Superconducting materials
    National Category
    Other Engineering and Technologies not elsewhere specified
    Identifiers
    urn:nbn:se:liu:diva-15068 (URN)10.1016/S0022-0248(01)02198-4 (DOI)
    Note
    The status of this article on the day of the defence was: Submitted and the title of the article was "Nitrogen doping of Silicon Carbide: Effect of Process Parameters"Available from: 2008-10-13 Created: 2008-10-13 Last updated: 2017-12-11Bibliographically approved
    7. Aluminum doping of epitaxial Silicon Carbide
    Open this publication in new window or tab >>Aluminum doping of epitaxial Silicon Carbide
    Show others...
    2003 (English)In: Journal of Crystal Growth, ISSN 0022-0248, E-ISSN 1873-5002, Vol. 253, no 1-4, p. 340-350Article in journal (Refereed) Published
    Abstract [en]

    Intentional doping of aluminum in 4H and 6H SiC has been performed using a hot-wall CVD reactor. The dependence of aluminum incorporation on temperature, pressure, C/Si ratio, growth rate, and TMA flow has been investigated. The aluminum incorporation showed to be polarity dependent. The high aluminum incorporation on the Si-face is closely related to the carbon coverage on the SiC surface. Changes in process parameters changes the effective C/Si ratio close to the SiC surface. Increased growth rate and C/Si ratio increases the aluminum incorporation on the Si-face. Diffusion limited incorporation occurs at high growth rate. Reduced pressure increases the effective C/Si ratio, and at low growth rate, the aluminum incorporation increases initially, levels off at a critical pressure, and continues to decrease below the critical pressure. The aluminum incorporation showed to be constant in a temperature range of 50°C. The highest atomic concentration of aluminum observed in this study was 3×1017 and 8×1018 cm−3 in Si and C-face, respectively.

    Place, publisher, year, edition, pages
    ScienceDirect, 2003
    Keywords
    A1. Doping; A1. Growth models; A3. Chemical vapor deposition processes; A3. Hot wall epitaxy; B2. Semiconducting silicon carbide
    National Category
    Other Engineering and Technologies not elsewhere specified
    Identifiers
    urn:nbn:se:liu:diva-15055 (URN)10.1016/S0022-0248(03)01045-5 (DOI)
    Note
    The status of the article on the defence day was: Submitted and the original title was "Aluminum doping of Silicon Carbide: Effect of Process Parameters".Available from: 2008-10-13 Created: 2008-10-13 Last updated: 2017-12-11Bibliographically approved
  • 47.
    Danielsson, Örjan
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
    Janzén, Erik
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
    Using N2 as precursor gas in III-nitride CVD growth2003In: Journal of Crystal Growth, ISSN 0022-0248, E-ISSN 1873-5002, Vol. 253, no 1-4, p. 26-37Article in journal (Refereed)
    Abstract [en]

    Computational fluid dynamics simulations have been performed to explore the possibility of using nitrogen gas as a precursor to III-nitride growth. A chemical model for the gas-phase decomposition of N2 has been used to show that large enough amounts of reactive species can be formed under conditions not far from those used in normal metalorganic chemical vapor deposition. Simulations were performed in 2D for various concentrations of N2, and comparisons with the use of NH3 were made. A modified reactor design needed to achieve high enough concentrations of reactive species is suggested. The possibility to increase the growth rate and material quality in III-nitride growth is discussed.

  • 48.
    Danielsson, Örjan
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
    Sukkaew, Pitsiri
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
    Ojamäe, Lars
    Linköping University, Department of Physics, Chemistry and Biology, Physical Chemistry. Linköping University, The Institute of Technology.
    Kordina, Olof
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
    Janzén, Erik
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
    Shortcomings of CVD modeling of SiC today2013In: Theoretical Chemistry accounts, ISSN 1432-881X, E-ISSN 1432-2234, Vol. 132, no 11, p. 1398-Article in journal (Refereed)
    Abstract [en]

    The active, epitaxial layers of silicon carbide (SiC) devices are grown by chemical vapor deposition (CVD), at temperatures above 1,600 °C, using silane and light hydrocarbons as precursors, diluted in hydrogen. A better understanding of the epitaxial growth process of SiC by CVD is crucial to improve CVD tools and optimize growth conditions. Through computational fluid dynamic (CFD) simulations, the process may be studied in great detail, giving insight to both flow characteristics, temperature gradients and distributions, and gas mixture composition and species concentrations throughout the whole CVD reactor. In this paper, some of the important parts where improvements are very much needed for accurate CFD simulations of the SiC CVD process to be accomplished are pointed out. First, the thermochemical properties of 30 species that are thought to be part of the gas-phase chemistry in the SiC CVD process are calculated by means of quantum-chemical computations based on ab initio theory and density functional theory. It is shown that completely different results are obtained in the CFD simulations, depending on which data are used for some molecules, and that this may lead to erroneous conclusions of the importance of certain species. Second, three different models for the gas-phase chemistry are compared, using three different hydrocarbon precursors. It is shown that the predicted gas-phase composition varies largely, depending on which model is used. Third, the surface reactions leading to the actual deposition are discussed. We suggest that hydrocarbon molecules in fact have a much higher surface reactivity with the SiC surface than previously accepted values.

  • 49.
    De Feudis, M.
    et al.
    University of Salento, Italy; INFN National Institute Nucl Phys, Italy.
    Caricato, A. P.
    University of Salento, Italy; INFN National Institute Nucl Phys, Italy.
    Taurino, A.
    CNR IMM Institute Microelect and Microsyst, Italy.
    Ossi, P. M.
    Politecn Milan, Italy.
    Castiglioni, C.
    Politecn Milan, Italy.
    Brambilla, L.
    Politecn Milan, Italy.
    Maruccio, G.
    NNL CNR Nanotec, Italy.
    Monteduro, A. G.
    NNL CNR Nanotec, Italy.
    Broitman, Esteban
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering.
    Chiodini, G.
    INFN National Institute Nucl Phys, Italy.
    Martino, M.
    University of Salento, Italy; INFN National Institute Nucl Phys, Italy.
    Diamond graphitization by laser-writing for all-carbon detector applications2017In: Diamond and related materials, ISSN 0925-9635, E-ISSN 1879-0062, Vol. 75, p. 25-33Article in journal (Refereed)
    Abstract [en]

    The surface of a detector grade CVD polycrystalline diamond sample (5 x 5 x 0.05 mm(3)) was irradiated by an ArF excimer laser (lambda = 193 nm, T = 20 ns) to produce graphitic conductive layers. In particular, two sets of four parallel graphitic strip-like contacts, with 1 mm pitch, were created along the whole sample on the top and on the rear surfaces of the sample respectively. The two series of stripes lie normally to each other. Such a grid allows to obtain a segmented all-carbon device capable of giving bi-dimensional information on particle detection processes in nuclear applications. Afterwards, an extensive characterization of the samples was performed: SEM and micro-Raman investigations to study the morphological and structural evolution of the irradiated areas, EDS measurements to individuate any absorption phenomena from environment associated to laser treatment, and nanoindentation mapping to understand how the hard-soft transformation occurred depending on the locally transferred energy. Finally, current-voltage analyses were carried out checking the ohmic behavior of the diamond-graphite contact. By comparing the results of the different characterization analyses, a strong periodidty of the modified surface properties was found, confirming the reliability and reproducibility of the laser-induced graphitization process. The results demonstrate that the laser-writing technique is a good and fast solution to produce graphitic contacts on diamond surface and therefore represents a promising way to fabricate segmented all-carbon devices. (C) 2016 Elsevier B.V. All rights reserved.

  • 50.
    Debela, Ahmed M.
    et al.
    Universitat Rovira i Virgili, Tarragona, Spain.
    Ortiz, Mayreli
    Universitat Rovira i Virgili, Tarragona, Spain.
    Beni, Valerio
    Universitat Rovira i Virgili, Tarragona, Spain.
    O´Sullivan, Ciara K.
    Universitat Rovira i Virgili, Tarragona, Spain and ICREA, Barcelona, Spain.
    Facile Electrochemical Hydrogenation and Chlorination of Glassy Carbon to Produce Highly Reactive and Uniform Surfaces for Stable Anchoring of Thiolated Molecules2014In: Chemistry - A European Journal, ISSN 0947-6539, Vol. 20, no 25, p. 7646-7654Article in journal (Refereed)
    Abstract [en]

    Carbon is a highly adaptable family of materials and is one of the most chemically stable materials known, providing a remarkable platform for the development of tunable molecular interfaces. Herein, we report a two-step process for the electrochemical hydrogenation of glassy carbon followed by either chemical or electrochemical chlorination to provide a highly reactive surface for further functionalization. The carbon surface at each stage of the process is characterized by AFM, SEM, Raman, attenuated total reflectance (ATR) FTIR, X-ray photoelectron spectroscopy (XPS), and electroanalytical techniques. Electrochemical chlorination of hydrogen-terminated surfaces is achieved in just 5 min at room temperature with hydrochloric acid, and chemical chlorination is performed with phosphorus pentachloride at 50 °C over a three-hour period. A more controlled and uniform surface is obtained using the electrochemical approach, as chemical chlorination is observed to damage the glassy carbon surface. A ferrocene-labeled alkylthiol is used as a model system to demonstrate the genericity and potential application of the highly reactive chlorinated surface formed, and the methodology is optimized. This process is then applied to thiolated DNA, and the functionality of the immobilized DNA probe is demonstrated. XPS reveals the covalent bond formed to be a CS bond. The thermal stability of the thiolated molecules anchored on the glassy carbon is evaluated, and is found to be far superior to that on gold surfaces. This is the first report on the electrochemical hydrogenation and electrochemical chlorination of a glassy carbon surface, and this facile process can be applied to the highly stable functionalization of carbon surfaces with a plethora of diverse molecules, finding widespread applications.

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