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  • 1.
    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.

    The full text will be freely available from 2020-04-24 11:07
  • 2.
    Colibaba, G. V
    et al.
    Moldova State Univ, Moldova.
    Avdonin, A.
    Polish Acad Sci, Poland.
    Shtepliuk, Ivan
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering. Frantsevich Inst Problems Mat Sci NASU, Ukraine.
    Caraman, M.
    Moldova State Univ, Moldova.
    Domagala, J.
    Polish Acad Sci, Poland.
    Inculet, I.
    Moldova State Univ, Moldova.
    Effects of impurity band in heavily doped ZnO:HCl2019In: Physica. B, Condensed matter, ISSN 0921-4526, E-ISSN 1873-2135, Vol. 553, p. 174-181Article in journal (Refereed)
    Abstract [en]

    A comparative study of properties of ZnO:HCl single crystals obtained by various methods is presented. Characterization by photoluminescence, optical and electrical measurements in the wide temperature range has allowed to analyze the energy spectra of Cl-containing stable defects in ZnO. Presence of shallow Cl donors, deeper donor complexes, incorporating several Cl atoms or stable H-Cl pairs and presence of compensating deep acceptors, attributed to VznClo centers, are demonstrated. The presence of shallow donor impurity band, as well as strong dependence of its activation energy on the doping level is shown. The controversy of various models for estimation of this dependence is discussed. It is demonstrated, that 90% of this dependence is caused by feature of temperature dependence of Hall coefficient related to conductive impurity band, and a more correct equation for activation energy is suggested. An abnormally low efficiency of neutral impurity scattering of charge carriers and strong optical absorption in the near-IR spectral range are demonstrated and attributed to upper conductive impurity band of negatively charged donors with an extra electron.

    The full text will be freely available from 2020-10-25 12:55
  • 3.
    Giannazzo, F.
    et al.
    CNR, Italy.
    Shtepliuk, Ivan
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Ivanov, Ivan Gueorguiev
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Iakimov, Tihomir
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Kakanakova-Gueorguieva, Anelia
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Schiliro, E.
    CNR, Italy.
    Fiorenza, P.
    CNR, Italy.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Probing the uniformity of hydrogen intercalation in quasi-free-standing epitaxial graphene on SiC by micro-Raman mapping and conductive atomic force microscopy2019In: Nanotechnology, ISSN 0957-4484, E-ISSN 1361-6528, Vol. 30, no 28, article id 284003Article in journal (Refereed)
    Abstract [en]

    In this paper, micro-Raman mapping and conductive atomic force microscopy (C-AFM) were jointly applied to investigate the structural and electrical homogeneity of quasi-free-standing monolayer graphene (QFMLG), obtained by high temperature decomposition of 4H-SiC(0001) followed by hydrogen intercalation at 900 degrees C. Strain and doping maps, obtained by Raman data, showed the presence of sub-micron patches with reduced hole density correlated to regions with higher compressive strain, probably associated with a locally reduced hydrogen intercalation. Nanoscale resolution electrical maps by C-AFM also revealed the presence of patches with enhanced current injection through the QFMLG/SiC interface, indicating a locally reduced Schottky barrier height (Phi(B)). The Phi(B) values evaluated from local I-V curves by the thermionic emission model were in good agreement with the values calculated for the QFMLG/SiC interface using the Schottky-Mott rule and the graphene holes density from Raman maps. The demonstrated approach revealed a useful and non-invasive method to probe the structural and electrical homogeneity of QFMLG for future nano-electronics applications.

  • 4.
    Ievtushenko, A.
    et al.
    NASU, Ukraine.
    Karpyna, V.
    NASU, Ukraine.
    Eriksson, Jens
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Tsiaoussis, I.
    Aristotle Univ Thessaloniki, Greece.
    Shtepliuk, Ivan
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering. NASU, Ukraine.
    Lashkarev, G.
    NASU, Ukraine.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Khranovskyy, Volodymyr
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Effect of Ag doping on the structural, electrical and optical properties of ZnO grown by MOCVD at different substrate temperatures2018In: Superlattices and Microstructures, ISSN 0749-6036, E-ISSN 1096-3677, Vol. 117, p. 121-131Article in journal (Refereed)
    Abstract [en]

    ZnO films and nanostructures were deposited on Si substrates by MOCVD using single source solid state zinc acetylacetonate (Zn(AA)) precursor. Doping by silver was realized in-situ via adding 1 and 10 wt. % of Ag acetylacetonate (Ag(AA)) to zinc precursor. Influence of Ag on the microstructure, electrical and optical properties of ZnO at temperature range 220-550 degrees C was studied by scanning, transmission electron and Kelvin probe force microscopy, photoluminescence and four-point probe electrical measurements. Ag doping affects the ZnO microstructure via changing the nucleation mode into heterogeneous and thus transforming the polycrystalline films into a matrix of highly c-axis textured hexagonally faceted nanorods. Increase of the work function value from 4.45 to 4.75 eV was observed with Ag content increase, which is attributed to Ag behaviour as a donor impurity. It was observed, that near-band edge emission of ZnO NS was enhanced with Ag doping as a result of quenching deep-level emission. Upon high doping of ZnO by Ag it tends to promote the formation of basal plane stacking faults defect, as it was observed by HR TEM and PL study in the case of 10 wt.% of Ag. Based on the results obtained, it is suggested that NS deposition at lower temperatures (220-300 degrees C) is more favorable for p-type doping of ZnO. (C) 2018 Elsevier Ltd. All rights reserved.

  • 5.
    Khomyak, V. V.
    et al.
    Fedkovich Chernivtsi National University, Ukraine.
    Ilashchuk, M. I.
    Fedkovich Chernivtsi National University, Ukraine.
    Shtepliuk, Ivan I.
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering. NAS Ukraine, Ukraine.
    Properties of p-n-junctions formed by a laser irradiation of a surface of n-Cd1-xZnx Te single crystal2015In: Semiconductor Science and Technology, ISSN 0268-1242, E-ISSN 1361-6641, Vol. 30, no 3, article id 035016Article in journal (Refereed)
    Abstract [en]

    Photosensitive barrier structures were fabricated by high-power pulsed laser irradiation of a freshly-cleaved surface of n-type bulk Cd1-xZnxTe substrates. Their electrical properties were investigated and discussed. Dominant carrier mechanisms at a forward and a reverse bias in terms of a recombination and tunnel-recombination model were analyzed. At the illumination reaching 100 mW.cm(-2), these surface-barrier p-Cd1-xZnxTe/n-Cd1-xZnxTe structures were possessed by the following photoelectric parameters: open-circuit voltage V-oc = 0.61 V, short-circuit current I-sc = 0.21 mA and fill factor FF = 0.49, respectively.

  • 6.
    Khranovskyy, Volodymyr
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Sendova, Mariana
    New Coll Florida, FL 34243 USA.
    Hosterman, Brian
    New Coll Florida, FL 34243 USA.
    McGinnis, Navin
    New Coll Florida, FL 34243 USA.
    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.
    Temperature dependent study of basal plane stacking faults in Ag:ZnO nanorods by Raman and photoluminescence spectroscopy2017In: Materials Science in Semiconductor Processing, ISSN 1369-8001, E-ISSN 1873-4081, Vol. 69, p. 62-67Article in journal (Refereed)
    Abstract [en]

    We report the specific features of basal plane stacking faults (BSFs) in ZnO nanorods (NRs), studied by temperature dependent photoluminescence and Raman spectroscopy. At low temperature (4 K) the intense band of emission at 3.321 eV is attributed to the presence of BSFs defects and Ag as an acceptor dopant in ZnO. This specific peak red-shifts with the temperature increase, occupying the position 3.210 eV at RT. The nature of the emission is explained as exciton recombination of the electrons, confined in the homo-heterojunction QW, with the holes, localized near the Ag atoms close to SFs. Raman spectroscopy revealed that Ag: ZnO nanorods have slightly downshifted positions of the modes 330 cm(-1) and 440 cm(-1) by 4 cm(-1), which we explain as due to the presence of BSFs. It was also observed, that the longitudinal optical phonon mode ALO, which is common polar mode for ZnO, was not detected by Raman spectroscopy in the samples with high BSFs density. This feature can be explained as due to existence of the bound charge induced by the BSFs in the NRs.

  • 7.
    Khranovskyy, Volodymyr
    et al.
    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.
    Ivanov, Ivan Gueorguiev
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Tsiaoussis, I.
    Aristotle University of Thessaloniki, Thessaloniki, Greece.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Light emission enhancement from ZnO nanostructured films grown on Gr/SiC substrates2016In: Carbon, ISSN 0008-6223, E-ISSN 1873-3891, Vol. 99, p. 295-301Article in journal (Refereed)
    Abstract [en]

    We report on the application of a single layer graphene substrates for the growth of polycrystalline ZnO films with advanced light emission properties. Unusually high ultraviolet (UV) and visible (VIS) photoluminesce was observed from the ZnO/Gr/SiC structures in comparison to identical samples without graphene. The photoluminescence intensity depends non-monotonically on the films thickness, reaching its maximum for 150 nm thick films. The phenomena observed is explained as due to the dual graphene role: i) the dangling bond free substrate, providing growth of relaxed thin ZnO layers ii) a back reflector active mirror of the Fabry-Perot cavity that is formed. The reported results demonstrate the potential of two-dimensional carbon materials integration with light emitting wide band gap semiconductors and can be of practical importance for the design of future optoelectronic devices.

  • 8.
    Khranovskyy, Volodymyr
    et al.
    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. Linköping University, Faculty of Science & Engineering. NAS Ukraine, Ukraine.
    Vines, L.
    UIO, Norway.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Complementary study of the photoluminescence and electrical properties of ZnO films grown on 4H-SiC substrates2017In: Journal of Luminescence, ISSN 0022-2313, E-ISSN 1872-7883, Vol. 181, p. 374-381Article in journal (Refereed)
    Abstract [en]

    We have studied the photoluminescence and electrical properties of ZnO films grown epitaxially by atmospheric pressure MOCVD on 4H-SiC substrates. The dominating DA line on the low temperature PL spectrum is attributed to the emission of an exciton bound to the neutral donor. The intensity of this line correlates with the electrical properties of the films: the decrease of DA intensity occurs simultaneously with the increase of the carriers mobility. This we explain as donor activation providing free electrons to the conduction band. Based on the comparison of the calculated value of donor binding energy, the literature data and complementary SIMS analysis a suggested donor impurity is aluminum (Al). The exciton localization energy is 16.3 meV, and agrees well with localization energy of 15.3 meV for Al impurity reported by other authors (e.g. Ref. [33]). The thermal activation energy E-D=22 meV, determined from the Hall data and is in agreement with the optical activation energy 20 meV, which is derived from the temperature-dependent PL study. The calculated value of the donor binding energy of 54.3 eV is in agreement with the ionization energy of 53 meV mentioned in earlier reports for Al in ZnO films. Our results prove that the commonly observed line at similar to 3.3599 eV on low temperature PL spectra of ZnO is a neutral donor bound exciton emission due to the Al impurity. (C) 2016 Elsevier B.V. All rights reserved.

  • 9.
    Rodner, Marius
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Puglisi, Donatella
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Ekeroth, Sebastian
    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.
    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.
    Skallberg, Andreas
    Linköping University, Department of Physics, Chemistry and Biology, Molecular Surface Physics and Nano Science. Linköping University, Faculty of Science & Engineering.
    Uvdal, Kajsa
    Linköping University, Department of Physics, Chemistry and Biology, Molecular Surface Physics and Nano Science. Linköping University, Faculty of Science & Engineering.
    Schutze, Andreas
    Saarland Univ, Germany.
    Eriksson, Jens
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Graphene Decorated with Iron Oxide Nanoparticles for Highly Sensitive Interaction with Volatile Organic Compounds2019In: Sensors, ISSN 1424-8220, E-ISSN 1424-8220, Vol. 19, no 4, article id 918Article in journal (Refereed)
    Abstract [en]

    Gases, such as nitrogen dioxide, formaldehyde and benzene, are toxic even at very low concentrations. However, so far there are no low-cost sensors available with sufficiently low detection limits and desired response times, which are able to detect them in the ranges relevant for air quality control. In this work, we address both, detection of small gas amounts and fast response times, using epitaxially grown graphene decorated with iron oxide nanoparticles. This hybrid surface is used as a sensing layer to detect formaldehyde and benzene at concentrations of relevance (low parts per billion). The performance enhancement was additionally validated using density functional theory calculations to see the effect of decoration on binding energies between the gas molecules and the sensor surface. Moreover, the time constants can be drastically reduced using a derivative sensor signal readout, allowing the sensor to work at detection limits and sampling rates desired for air quality monitoring applications.

  • 10.
    Santangelo, Francesca
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Shtepliuk, Ivan
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Filippini, Daniel
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Ivanov, Ivan Gueorguiev
    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.
    Eriksson, Jens
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Real-time sensing of lead with epitaxial graphene-integrated microfluidic devices2019In: Sensors and actuators. B, Chemical, ISSN 0925-4005, E-ISSN 1873-3077, Vol. 288, p. 425-431Article in journal (Refereed)
    Abstract [en]

    Since even low concentrations of toxic heavy metals can seriously damage human health, it is important to develop simple, sensitive and accurate methods for their detection. Graphene, which is extremely sensitive to foreign species, is a key element in the development of a sensing platform where low concentrations of analyte have to be detected. This work discusses the proof of concept of a sensing platform for liquid-phase detection of heavy metals (e.g. Pb) based on epitaxial graphene sensors grown on Si-face 4H-SiC substrate (EG/SiC). The sensing platform developed includes a microfluidic chip incorporating all the features needed to connect and execute the Lab-on-chip (LOC) functions using 3D printing fast prototyping technology. Herein, we present the response of EG to concentrations of Pb2+ solutions ranging from 125 nM to 500 mu M, showing good stability and reproducibility over time and an enhancement of its conductivity with a Langmuir correlation between signal and Pb2+ concentration. Density functional theory (DFT) calculations are performed and clearly explain the conductivity changes and the sensing mechanism in agreement with the experimental results reported, confirming the strong sensitivity of the sensor to the lowest concentrations of the analyte. Furthermore, from the calibration curve of the system, a limit of detection (LoD) of 95 nM was extrapolated.

  • 11.
    Santangelo, Francesca
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Shtepliuk, Ivan
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Filippini, Daniel
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Puglisi, Donatella
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Eriksson, Jens
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Epitaxial Graphene Sensors Combined with 3D-Printed Microfluidic Chip for Heavy Metals Detection2019In: Sensors, ISSN 1424-8220, E-ISSN 1424-8220, Vol. 19, no 10, article id 2393Article in journal (Refereed)
    Abstract [en]

    In this work, we investigated the sensing performance of epitaxial graphene on Si-face 4H-SiC (EG/SiC) for liquid-phase detection of heavy metals (e.g., Pb and Cd), showing fast and stable response and low detection limit. The sensing platform proposed includes 3D-printed microfluidic devices, which incorporate all features required to connect and execute lab-on-chip (LOC) functions. The obtained results indicate that EG exhibits excellent sensing activity towards Pb and Cd ions. Several concentrations of Pb2+ solutions, ranging from 125 nM to 500 mu M, were analyzed showing Langmuir correlation between signal and Pb2+ concentrations, good stability, and reproducibility over time. Upon the simultaneous presence of both metals, sensor response is dominated by Pb2+ rather than Cd2+ ions. To explain the sensing mechanisms and difference in adsorption behavior of Pb2+ and Cd2+ ions on EG in water-based solutions, we performed van-der-Waals (vdW)-corrected density functional theory (DFT) calculations and non-covalent interaction (NCI) analysis, extended charge decomposition analysis (ECDA), and topological analysis. We demonstrated that Pb2+ and Cd2+ ions act as electron-acceptors, enhancing hole conductivity of EG, due to charge transfer from graphene to metal ions, and Pb2+ ions have preferential ability to binding with graphene over cadmium. Electrochemical measurements confirmed the conductometric results, which additionally indicate that EG is more sensitive to lead than to cadmium.

  • 12.
    Santangelo, Maria Francesca
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Shtepliuk, Ivan I.
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Puglisi, Donatella
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Filippini, Daniel
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Eriksson, Jens
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Epitaxial graphene sensors combined with 3D printed microfluidic chip for heavy metals detection2018In: Proceedings, ISSN 2504-3900, Vol. 2, no 13, article id 982Article in journal (Refereed)
    Abstract [en]

    Two-dimensional materials may constitute key elements in the development of a sensing platform where extremely high sensitivity is required, since even minimal chemical interaction can generate appreciable changes in the electronic state of the material. In this work, we investigate the sensing performance of epitaxial graphene on Si-face 4H-SiC (EG/SiC) for liquid-phase detection of heavy metals (e.g., Pb). The integration of preparatory steps needed for sample conditioning is included in the sensing platform, exploiting fast prototyping using a 3D printer, which allows direct fabrication of a microfluidic chip incorporating all the features required to connect and execute the Lab-on-chip (LOC) functions. It is demonstrated that interaction of Pb2+ ions in water-based solutions with the EG enhances its conductivity exhibiting a Langmuir correlation between signal and Pb2+ concentration. Several concentrations of Pb2+ solutions ranging from 125 nM to 500 µM were analyzed showing good stability and reproducibility over time.

  • 13.
    Shavanova, Kateryna
    et al.
    National University of Life and Environm Science Ukraine, Ukraine.
    Bakakina, Yulia
    National Academic Science Belarus, Byelarus.
    Burkova, Inna
    National University of Life and Environm Science Ukraine, Ukraine.
    Shtepliuk, Ivan
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering.
    Viter, Roman
    University of Latvia, Latvia.
    Ubelis, Arnolds
    University of Latvia, Latvia.
    Beni, Valerio
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering.
    Starodub, Nickolaj
    National University of Life and Environm Science Ukraine, Ukraine.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Khranovskyy, Volodymyr
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Application of 2D Non-Graphene Materials and 2D Oxide Nanostructures for Biosensing Technology2016In: Sensors, ISSN 1424-8220, E-ISSN 1424-8220, Vol. 16, no 2Article, review/survey (Refereed)
    Abstract [en]

    The discovery of graphene and its unique properties has inspired researchers to try to invent other two-dimensional (2D) materials. After considerable research effort, a distinct "beyond graphene" domain has been established, comprising the library of non-graphene 2D materials. It is significant that some 2D non-graphene materials possess solid advantages over their predecessor, such as having a direct band gap, and therefore are highly promising for a number of applications. These applications are not limited to nano- and opto-electronics, but have a strong potential in biosensing technologies, as one example. However, since most of the 2D non-graphene materials have been newly discovered, most of the research efforts are concentrated on material synthesis and the investigation of the properties of the material. Applications of 2D non-graphene materials are still at the embryonic stage, and the integration of 2D non-graphene materials into devices is scarcely reported. However, in recent years, numerous reports have blossomed about 2D material-based biosensors, evidencing the growing potential of 2D non-graphene materials for biosensing applications. This review highlights the recent progress in research on the potential of using 2D non-graphene materials and similar oxide nanostructures for different types of biosensors (optical and electrochemical). A wide range of biological targets, such as glucose, dopamine, cortisol, DNA, IgG, bisphenol, ascorbic acid, cytochrome and estradiol, has been reported to be successfully detected by biosensors with transducers made of 2D non-graphene materials.

  • 14.
    Shtepliuk, Ivan
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering. NASU, Ukraine.
    Caffrey, Nuala M.
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering. Trinity Coll Dublin, Ireland; Trinity Coll Dublin, Ireland.
    Iakimov, Tihomir
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Khranovskyy, Volodymyr
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Abrikosov, Igor
    Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics. Linköping University, Faculty of Science & Engineering. National University of Science and Technology MISIS, Russia.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    On the interaction of toxic Heavy Metals (Cd, Hg, Pb) with graphene quantum dots and infinite graphene2017In: Scientific Reports, ISSN 2045-2322, E-ISSN 2045-2322, Vol. 7, article id 3934Article in journal (Refereed)
    Abstract [en]

    The promise of graphene and its derivatives as next generation sensors for real-time detection of toxic heavy metals (HM) requires a clear understanding of behavior of these metals on the graphene surface and response of the graphene to adsorption events. Our calculations herein were focused on the investigation of the interaction between three HMs, namely Cd, Hg and Pb, with graphene quantum dots (GQDs). We determine binding energies and heights of both neutral and charged HM ions on these GQDs. The results show that the adsorption energy of donor-like physisorbed neutral Pb atoms is larger than that of either Cd or Hg. In contrast to the donor-like behavior of elemental HMs, the chemisorbed charged HM species act as typical acceptors. The energy barriers to migration of the neutral adatoms on GQDs are also estimated. In addition, we show how the substitution of a carbon atom by a HM adatom changes the geometric structure of GQDs and hence their electronic and vibrational properties. UV-visible absorption spectra of HM-adsorbed GQDs vary with the size and shape of the GQD. Based on our results, we suggest a route towards the development of a graphene-based sensing platform for the optical detection of toxic HMs.

  • 15.
    Shtepliuk, Ivan
    et al.
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering.
    Eriksson, Jens
    Linköping University, Department of Physics, Chemistry and Biology, Applied Sensor Science. Linköping University, Faculty of Science & Engineering.
    Khranovskyy, Volodymyr
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Iakimov, Tihomir
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Lloyd Spetz, Anita
    Linköping University, Department of Physics, Chemistry and Biology, Applied Sensor Science. Linköping University, Faculty of Science & Engineering.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Monolayer graphene/SiC Schottky barrier diodes with improved barrier height uniformity as a sensing platform for the detection of heavy metals2016In: Beilstein Journal of Nanotechnology, ISSN 2190-4286, Vol. 7, p. 1800-1814Article in journal (Refereed)
    Abstract [en]

    A vertical diode structure comprising homogeneous monolayer epitaxial graphene on silicon carbide is fabricated by thermal decomposition of a Si-face 4H-SiC wafer in argon atmosphere. Current-voltage characteristics of the graphene/SiC Schottky junction were analyzed by applying the thermionic-emission theory. Extracted values of the Schottky barrier height and the ideality factor are found to be 0.4879 +/- 0.013 eV and 1.01803 +/- 0.0049, respectively. Deviations of these parameters from average values are smaller than those of previously observed literature data, thereby implying uniformity of the Schottky barrier height over the whole diode area, a stable rectifying behaviour and a good quality of ohmic palladium-graphene contacts. Keeping in mind the strong sensitivity of graphene to analytes we propose the possibility to use the graphene/SiC Schottky diode as a sensing platform for the recognition of toxic heavy metals. Using density functional theory (DFT) calculations we gain insight into the nature of the interaction of cadmium, mercury and lead with graphene as well as estimate the work function and the Schottky barrier height of the graphene/SiC structure before and after applying heavy metals to the sensing material. A shift of the I-V characteristics of the graphene/SiC-based sensor has been proposed as an indicator of presence of the heavy metals. Since the calculations suggested the strongest charge transfer between Pb and graphene, the proposed sensing platform was characterized by good selectivity towards lead atoms and slight interferences from cadmium and mercury. The dependence of the sensitivity parameters on the concentration of Cd, Hg and Pb is studied and discussed.

  • 16.
    Shtepliuk, Ivan I.
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering. NASU, Ukraine.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Ivanov, Ivan Gueorguiev
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Iakimov, Tihomir
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Yazdi, Gholamreza
    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.
    Lead (Pb) interfacing with epitaxial graphene2018In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 20, no 25, p. 17105-17116Article in journal (Refereed)
    Abstract [en]

    Here, we report the electrochemical deposition of lead (Pb) as a model metal on epitaxial graphene fabricated on silicon carbide (Gr/SiC). The kinetics of electrodeposition and morphological characteristics of the deposits were evaluated by complementary electrochemical, physical and computational methods. The use of Gr/SiC as an electrode allowed the tracking of lead-associated redox conversions. The analysis of current transients passed during the deposition revealed an instantaneous nucleation mechanism controlled by convergent mass transport on the nuclei locally randomly distributed on epitaxial graphene. This key observation of the deposit topology was confirmed by low values of the experimentally-estimated apparent diffusion coefficient, Raman spectroscopy and scanning electron microscopy (SEM) studies. First principles calculations showed that the nucleation of Pb clusters on the graphene surface leads to weakening of the interaction strength of the metal-graphene complex, and only spatially separated Pb adatoms adsorbed on bridge and/or edge-plane sites can affect the vibrational properties of graphene. We expect that the lead adatoms can merge in large metallic clusters only at defect sites that reinforce the metal-graphene interactions. Our findings provide valuable insights into both heavy metal ion electrochemical analysis and metal electroplating on graphene interfaces that are important for designing effective detectors of toxic heavy metals.

  • 17.
    Shtepliuk, Ivan
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Iakimov, Tihomir
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Khranovskyy, Volodymyr
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Eriksson, Jens
    Linköping University, Department of Physics, Chemistry and Biology, Applied Sensor Science. Linköping University, Faculty of Science & Engineering.
    Giannazzo, Filippo
    CNR IMM, Italy.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Role of the Potential Barrier in the Electrical Performance of the Graphene/SiC Interface2017In: Crystals, ISSN 2073-4352, Vol. 7, no 6, article id 162Article, review/survey (Refereed)
    Abstract [en]

    In spite of the great expectations for epitaxial graphene (EG) on silicon carbide (SiC) to be used as a next-generation high-performance component in high-power nano- and micro-electronics, there are still many technological challenges and fundamental problems that hinder the full potential of EG/SiC structures and that must be overcome. Among the existing problems, the quality of the graphene/SiC interface is one of the most critical factors that determines the electroactive behavior of this heterostructure. This paper reviews the relevant studies on the carrier transport through the graphene/SiC, discusses qualitatively the possibility of controllable tuning the potential barrier height at the heterointerface and analyses how the buffer layer formation affects the electronic properties of the combined EG/SiC system. The correlation between the sp(2)/sp(3) hybridization ratio at the interface and the barrier height is discussed. We expect that the barrier height modulation will allow realizing a monolithic electronic platform comprising different graphene interfaces including ohmic contact, Schottky contact, gate dielectric, the electrically-active counterpart in p-n junctions and quantum wells.

  • 18.
    Shtepliuk, Ivan
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Ivanov, Ivan Gueorguiev
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Iakimov, Tihomir
    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.
    Kakanakova-Gueorguieva, Anelia
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Fiorenza, Patrick
    CNR IMM, Italy.
    Giannazzo, Filippo
    CNR IMM, Italy.
    Raman probing of hydrogen-intercalated graphene on Si-face 4H-SiC2019In: Materials Science in Semiconductor Processing, ISSN 1369-8001, E-ISSN 1873-4081, Vol. 96, p. 145-152Article in journal (Refereed)
    Abstract [en]

    We report the results of in-depth Raman study of quasi-free-standing monolayer graphene on the (0001) Si- face of 4H-SiC, which contains similar to 0.1-2.10(11) cm(-2) sp(3) defects that have been introduced by hydrogen intercalation. The nature of the intercalation-induced defects is elucidated and ascribed to the formation of the C-H bonds. At the higher intercalation temperature in the formed monolayer graphene the defect-related Raman scattering displays a great enhancement and new spectral features attributed to D and D+D modes appear. Comprehensive statistical analysis of the Raman data enabled us to estimate the homogeneity of the Raman scattering processes and to separate strain and doping effects. Analysis of the compressive strain and carrier density maps revealed that the intercalation temperature of 900 degrees C and intercalation time of 1 h are more favorable conditions for conversion of the buffer layer to uniformly relaxed and p-doped monolayer graphene in comparison to annealing at 1100 degrees C for 30 min.

    The full text will be freely available from 2021-03-04 17:19
  • 19.
    Shtepliuk, Ivan
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering. NASU, Ukraine.
    Ivanov, Ivan Gueorguiev
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Pliatsikas, Nikolaos
    Linköping University, Department of Physics, Chemistry and Biology, Nanoscale engineering. Linköping University, Faculty of Science & Engineering.
    Ben Sedrine, N.
    Univ Aveiro, Portugal; Univ Aveiro, Portugal.
    Andersson, O.
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering.
    Iakimov, Tihomir
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Jamnig, Andreas
    Linköping University, Department of Physics, Chemistry and Biology, Nanoscale engineering. Linköping University, Faculty of Science & Engineering.
    Sarakinos, Kostas
    Linköping University, Department of Physics, Chemistry and Biology, Nanoscale engineering. Linköping University, Faculty of Science & Engineering.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Interplay between thin silver films and epitaxial graphene2020In: Surface & Coatings Technology, ISSN 0257-8972, E-ISSN 1879-3347, Vol. 381, article id 125200Article in journal (Refereed)
    Abstract [en]

    Thin Ag films, with nominal thickness in the range 2 to 30 nm, are deposited using direct current magnetron sputtering and film morphology is studied by means of plan-view scanning electron microscopy. We find that for 2 mn nominal thickness the film surface consists of isolated circular nanoscale islands, which become interconnected as further material is deposited, leading to a continuous film at a nominal thickness of 30 nm. Our experimental findings are discussed in the context of the density functional theory results, which show that van der Waals forces dominate the interaction between Ag and epitaxial graphene. We also performed micro-Raman analysis and we find that the G and 2D modes of epitaxial graphene exhibit a red-shift upon Ag-layer deposition; which is interpreted as a result of charge transfer at the Ag/graphene interface. Moreover, we observed a pronounced enhancement of the G peak amplitude and area irrespective of the film nominal thickness and morphology, which we attribute to a combination of the charge transfer and plasmonic resonance effects. Our observations provide a critical information on the interaction between Ag and epitaxial graphene, which can be useful to design electronic and sensing devices based on Ag-epitaxial graphene hybrids.

    The full text will be freely available from 2021-11-28 13:48
  • 20.
    Shtepliuk, Ivan
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering. Natl Acad Sci Ukraine, Ukraine.
    Ivanov, Ivan Gueorguiev
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Pliatsikas, Nikolaos
    Linköping University, Department of Physics, Chemistry and Biology, Nanoscale engineering. Linköping University, Faculty of Science & Engineering.
    Iakimov, Tihomir
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Jamnig, Andreas
    Linköping University, Department of Physics, Chemistry and Biology, Nanoscale engineering. Linköping University, Faculty of Science & Engineering.
    Sarakinos, Kostas
    Linköping University, Department of Physics, Chemistry and Biology, Nanoscale engineering. Linköping University, Faculty of Science & Engineering.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Probing the uniformity of silver-doped epitaxial graphene by micro-Raman mapping2020In: Physica. B, Condensed matter, ISSN 0921-4526, E-ISSN 1873-2135, Vol. 580, article id 411751Article in journal (Refereed)
    Abstract [en]

    We present a Raman spectroscopy study on epitaxial graphene decorated with thin Ag films (2-15 nm), which are deposited using magnetron sputtering. We find that the presence of Ag on the graphene surface induces doping, the uniformity and efficiency of which is determined by Ag nominal thickness. Deposition of Ag films with thicknesses up to 5 nm favors the effective electron transfer from Ag to epitaxial graphene. A significant redshift and broadening of the 2D peak are observed with increasing the Ag-layer thickness above 5 nm, which is indicative of large strain and doping fluctuations. We also observe a non-trivial linear growth of 2D/G peak intensity ratio with increasing D/G ratio for all Ag-decorated samples, which is explained by increase of peak amplitude due to surface enhanced Raman scattering and charged impurity-induced screening caused by the presence of Ag on the graphene surface.

    The full text will be freely available from 2021-10-07 15:40
  • 21.
    Shtepliuk, Ivan
    et al.
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering. Frantsevich Institute Problems Mat Science NAS Ukraine, Ukraine.
    Khranovskyy, Volodymyr
    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.
    Effect of c-axis inclination angle on the properties of ZnO/Zn1-xCdxO/ZnO quantum wells2016In: Thin Solid Films, ISSN 0040-6090, E-ISSN 1879-2731, Vol. 603, p. 139-148Article in journal (Refereed)
    Abstract [en]

    The development of optoelectronic devices based on highly-promising Zn1 - xCdxO semiconductor system demands deep understanding of the properties of the Zn1 - xCdxO-based quantum wells (QWs). In this regard, we carried out a numerical study of the polarization-related effects in polar, semi-polar and non-polar ZnO/ Zn1 - xCd xO/ZnO QWs with different parameters of the quantum well structure. The effects of well width, barrier thickness, cadmium content in the active layer and c-axis inclination angle on the distribution of the electron and hole wave function and transition energy were investigated using the 6 x 6 k center dot p Hamiltonian and one-dimensional self-consistent solutions of nonlinear Schrodinger-Poisson equations with consideration of spatially varying dielectric constant and effective mass. The strong sensitivity of the internal electric field, transition energy and overlap integral to cadmium content and well thickness in the angle range from 0 to 40 degrees was revealed. An unexpected change of the internal electric fields sign was observed at the angles ranging from 70 to 90 degrees. We also found a difference in the electronic properties between (0001)-, (11 (2) over bar2)-and (10 (1) over bar0)-oriented QWs.

  • 22.
    Shtepliuk, Ivan
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering. NASU, Ukraine.
    Khranovskyy, Volodymyr
    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.
    Insights into the origin of the excited transitions in graphene quantum dots interacting with heavy metals in different media2017In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 19, no 45, p. 30445-30463Article in journal (Refereed)
    Abstract [en]

    Exploring graphene quantum dots (GQDs) is an attractive way to design novel optical and electrochemical sensors for fast and reliable detection of toxic heavy metals (HMs), such as Cd, Hg and Pb. There are two main strategies for achieving this: (i) surface modification of an electrochemical working electrode by nanoscale GQDs and (ii) using a GQD solution electrolyte for optical sensing. Further development of these sensing technologies towards reaching or exceeding the WHO permissible limits implies deep understanding of the interaction between GQDs and HMs in different dielectric media. Solvent is expected to be one of the key factors affecting the binding ability of the GQDs to HMs and their electronic and optical properties. Here we show that the solvent-solute interaction changes the geometrical configuration, stability and absorption spectra of zigzag/armchair-edged GQDs after complexation with neutral and charged HM species. We observe physisorption behavior of Cd and Hg adatoms on the sp(2) surface with a solvent-mediated enhancement of the binding energy with increasing solvent polarity. For Pb adatoms, an opposite picture is revealed. We find that the solvent effect also manifests itself in weakening of the chemisorption strength in the HM cation-pi system with increasing dielectric constant of the solvent. Thus, a solvent engineering strategy based on control of the dielectric permittivity can be a promising approach to reach the desired binding energy in the HM@GQDs and to provide high sensitivity and selectivity of both optical and electrochemical sensors to toxic HMs we are interested in.

  • 23.
    Shtepliuk, Ivan
    et al.
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering.
    Khranovskyy, Volodymyr
    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.
    Theoretical study of O- and Zn-face polarity effect on the optical properties of the conventional and staggered ZnO/Zn1-xCdxO/ZnO quantum wells2015In: Thin Solid Films, ISSN 0040-6090, E-ISSN 1879-2731, Vol. 594, p. 323-327Article in journal (Refereed)
    Abstract [en]

    In this work we present a comparative study of Zn-face and O-face polarity Zn1 - xCdxO-based conventional and staggered quantum-well (QW) structures. The calculation of optical properties of QWs was performed by means of self-consistent Schrodinger-Poisson solver with consideration of polarization-induced effects. The conventional Zn-face and O-face QWs possess similar values of transition energy and an overlap of electron and hole wave functions. A change of the polarity from Zn-face to O-face for the conventional QWs influences only a shape of the conduction and valence band edge profile. It is revealed that the utilization of the staggered QWs leads to an improvement of the confinement characteristics. In addition, the O-face staggered QW structure has larger values of transition energy and overlap integral compared to the Zn-face staggered QW structure. O-terminated staggered QW structure is less dependent on the well thickness and has lower sensitivity to Cd content in embedded Zn1 - xCdxO layer. Control of the material polarity and design of the staggered QWs provide cost-effective approach for engineering the QW band structures with enhanced QW performance. This enables constructing of the Zn1 - xCdxO-based light emission diodes with improved radiative efficiency emitting, applicable for solid state lighting. (C) 2015 Elsevier B.V. All rights reserved.

  • 24.
    Shtepliuk, Ivan
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering. NASU, Ukraine.
    Santangelo, Maria Francesca
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Ivanov, Ivan Gueorguiev
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Khranovskyy, Volodymyr
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Iakimov, Tihomir
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Eriksson, Jens
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Understanding Graphene Response to Neutral and Charged Lead Species: Theory and Experiment2018In: Materials, ISSN 1996-1944, E-ISSN 1996-1944, Vol. 11, no 10, article id 2059Article in journal (Refereed)
    Abstract [en]

    Deep understanding of binding of toxic Lead (Pb) species on the surface of two-dimensional materials is a required prerequisite for the development of next-generation sensors that can provide fast and real-time detection of critically low concentrations. Here we report atomistic insights into the Lead behavior on epitaxial graphene (Gr) on silicon carbide substrates by thorough complementary study of voltammetry, electrical characterization, Raman spectroscopy, and Density Functional Theory (DFT). It is verified that the epitaxial graphene exhibits quasi-reversible anode reactions in aqueous solutions, providing a well-defined redox peak for Pb species and good linearity over a concentration range from 1 nM to 1 mu M. The conductometric approach offers another way to investigate Lead adsorption, which is based on the formations of stable charge-transfer complexes affecting the p-type conductivity of epitaxial graphene. Our results suggest the adsorption ability of the epitaxial graphene towards divalent Lead ions is concentration-dependent and tends to saturate at higher concentrations. To elucidate the mechanisms responsible for Pb adsorption, we performed DFT calculations and estimated the solvent-mediated interaction between Lead species in different oxidative forms and graphene. Our results provide central information regarding the energetics and structure of Pb-graphene interacting complexes that underlay the adsorption mechanisms of neutral and divalent Lead species. Such a holistic understanding favors design and synthesis of new sensitive materials for water quality monitoring.

  • 25.
    Shtepliuk, Ivan
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering. NASU, Kyiv, Ukraine.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. 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.
    Insights into the Electrochemical Behavior of Mercury on Graphene/SiC Electrodes2019In: C — Journal of Carbon Research, ISSN 2311-5629, Vol. 5, no 3, article id 51Article in journal (Refereed)
    Abstract [en]

    Fast and real time detection of Mercury (Hg) in aqueous solutions is a great challenge due to its bio-accumulative character and the detrimental effect on human health of this toxic element. Therefore, development of reliable sensing platforms is highly desirable. Current research is aiming at deep understanding of the electrochemical response of epitaxial graphene to Mercury exposure. By performing cyclic voltammetry and chronoamperometry measurements as well as density functional theory calculations, we elucidate the nature of Hg-involved oxidation-reduction reactions at the graphene electrode and shed light on the early stages of Hg electrodeposition. The obtained critical information of Hg behavior will be helpful for the design and processing of novel graphene-based sensors.

  • 26.
    Shtepliuk, Ivan
    et al.
    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.
    Interaction of epitaxial graphene with heavy metals: towards novel sensing platform2019In: Nanotechnology, ISSN 0957-4484, E-ISSN 1361-6528, Vol. 30, no 29, article id 294002Article in journal (Refereed)
    Abstract [en]

    Development of next-generation sensors based on graphene materials, especially epitaxial graphene (EG) as the most promising representative, with desirable cross-reactivity to heavy metals (HMs) is of great technological significance in the virtue of enormous impact on environmental sensorics. Nevertheless, the mechanisms by which EG responds to toxic HMs exposure and then produces the output signal are still obscure. In the present study, the nature of interaction of toxic HMs, e.g. Cd, Hg and Pb in neutral charge state and EG on Si-face SiC in the absence and in the presence of pure water solution has been investigated using density functional theory with the inclusion of dispersion correction and cluster model of EG. The gas-phase calculations showed that adsorbed electron-donating Cd and Hg adatoms on EG are most stable when bonded to hollow sites, while Pb species prefer to sit above bridge sites. By using non-covalent interaction analysis, charge decomposition analysis, overlap population density of states analysis and topological analysis, it was found that the interaction between Cd or Hg and EG is non-bonding in nature and is mainly governed by van der Waals forces, while Pb adsorption is followed by the formation of anti-bonding orbitals in vacuum conditions and bonding orbitals in water. The role of solvent in the adsorption behavior of HMs is studied and discussed. The present theoretical analysis is in good agreement with recent experimental results towards discriminative electrochemical analysis of the toxic HMs in aqueous solutions at critically low concentrations.

  • 27.
    Shtepliuk, Ivan
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering. NASU, Ukraine.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Interband Absorption in Few-Layer Graphene Quantum Dots: Effect of Heavy Metals2018In: Materials, ISSN 1996-1944, E-ISSN 1996-1944, Vol. 11, no 7, article id 1217Article in journal (Refereed)
    Abstract [en]

    Monolayer, bilayer, and trilayer graphene quantum dots (GQDs) with different binding abilities to elemental heavy metals (HMs: Cd, Hg, and Pb) were designed, and their electronic and optical properties were investigated theoretically to understand deeply the optical response under heavy metal exposure. To gain insight into the nature of interband absorption, we performed density functional theory (DFT) and time-dependent density functional theory (TD-DFT) calculations for thickness-varying GQDs. We found that the interband absorption in GQDs can be efficiently tuned by controlling the thickness of GQDs to attain the desirable coloration of the interacting complex. We also show that the strength of the interaction between GQDs and Cd, Hg, and Pb is strongly dependent on the number of sp(2)-bonded layers. The results suggest that the thickness of GQDs plays an important role in governing the hybridization between locally-excited (LE) and charge-transfer (CT) states of the GQDs. Based on the partial density-of-states (DOS) analysis and in-depth knowledge of excited states, the mechanisms underlying the interband absorption are discussed. This study suggests that GQDs would show an improved sensing performance in the selective colorimetric detection of lead by the thickness control.

  • 28.
    Shtepliuk, Ivan
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering. NASU, Ukraine.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Interband transitions in closed-shell vacancy containing graphene quantum dots complexed with heavy metals2018In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 20, no 33, p. 21528-21543Article in journal (Refereed)
    Abstract [en]

    High-performance optical detection of toxic heavy metals by using graphene quantum dots (GQDs) requires a strong interaction between the metals and GQDs, which can be reached through a functionalization/immobilization procedure or doping effect. However, commonly used surface activation approaches induce toxicity into the analysis system and, therefore, are ineligible from the environmental point of view. Here, we show that artificial creation of vacancy-type defects in GQDs can be a helpful means of intentional control of the active sites available for reaction with cadmium (Cd), mercury (Hg) and lead (Pb). Using restricted density functional theory (DFT) and time-dependent DFT (TD-DFT) methods, we predict the effect of vacancy complexes not previously studied to describe the binding ability of GQDs towards metal adsorbates. We also show that the interband absorption in closed-shell GQDs complexed with Cd, Hg and Pb is strongly dependent on the vacancy type and can be efficiently tuned to attain the desired coloration of the analysis system. The results suggest that the vacancy defects play an important role in governing the hybridization between locally-excited (LE) and charge-transfer (CT) states of the GQDs. Based on the molecular orbital analysis and in-depth knowledge of excited states, the mechanisms underlying the interband absorption are discussed.

  • 29.
    Yazdi, Gholamreza
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Akhtar, Fatima
    IHP, Germany.
    Ivanov, Ivan Gueorguiev
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Schmidt, Susann
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Shtepliuk, Ivan
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Zakharov, Alexei
    Lund Univ, Sweden.
    Iakimov, Tihomir
    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.
    Effect of epitaxial graphene morphology on adsorption of ambient species2019In: Applied Surface Science, ISSN 0169-4332, E-ISSN 1873-5584, Vol. 486, p. 239-248Article in journal (Refereed)
    Abstract [en]

    This work illustrates the impact of atmospheric gases on the surface of epitaxial graphene. The different rate of adsorption on different parts of graphene samples provides a concrete evidence that the surface morphology of graphene plays a significant role in this process. The uneven adsorption occurs only on the surface of the monolayer graphene and not on bilayer graphene. The second monolayer is distinguished and verified by the phase contrast mode of atomic force microscopy and the low energy electron microscopy, respectively. Raman spectroscopy is used to study the strain on the surface of graphene; results indicate that monolayer and bilayer graphene exhibit different types of strain. The bilayer is under more compressive strain in comparison with monolayer graphene that hinders the process of adsorption. However, the wrinkles and edges of steps of the bilayer are under tensile strain, hence, facilitate adsorption. Samples were subjected to X-ray photoelectron spectroscopy which confirms that the adsorbates on the epitaxial graphene are carbon clusters with nitrogen and oxygen contamination. For reversing the adsorption process the samples are annealed and a method for the removal of these adsorbates is proposed.

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