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  • 101.
    Lindell, Linda
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, The Institute of Technology.
    Burquel, A.
    Service de Chimie des Matériaux Nouveaux, Université de Mons-Hainaut, Place du Parc 20, 5-7000 Mons, Belgium.
    Jakobsson, Fredrik
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Lemaur, V.
    Service de Chimie des Matériaux Nouveaux, Université de Mons-Hainaut, Place du Parc 20, 5-7000 Mons, Belgium.
    Berggren, Magnus
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Lazzaroni, R.
    Service de Chimie des Matériaux Nouveaux, Université de Mons-Hainaut, Place du Parc 20, 5-7000 Mons, Belgium.
    Cornil, J.
    Service de Chimie des Matériaux Nouveaux, Université de Mons-Hainaut, Place du Parc 20, 5-7000 Mons, Belgium.
    Salaneck, William R
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, The Institute of Technology.
    Crispin, Xavier
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Transparent, plastic, low-work-function poly(3,4-ethylenedioxythiophene) electrodes2006In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 18, no 18, p. 4246-4252Article in journal (Refereed)
    Abstract [en]

    Novel applications for flexible electronics, e.g., displays and solar cells, require fully flexible, transparent, stable, and low-work-function electrodes that can be manufactured via a low-cost process. Here, we demonstrate that surface chemistry constitutes a route to producing transparent low-work-function plastic electrodes. The work function of the conducting polymer poly(3,4-ethylenedioxythiophene)-tosylate, or PEDOT-Tos, is decreased by submonolayer surface redox reaction with a strong electron donor, tetrakis-(dimethylamino)ethylene (TDAE), allowing it to reach a work function of 3.8 eV. The interface formed between TDAE and PEDOT is investigated in a joint experimental and theoretical study using photoelectron spectroscopy and quantum chemical calculations. © 2006 American Chemical Society.

  • 102.
    Lindell, Linda
    et al.
    Linköping University, The Institute of Technology. Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry.
    de Jong, Michel P
    Linköping University, The Institute of Technology. Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry.
    Osikowicz, Wojciech
    Linköping University, The Institute of Technology. Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry.
    Lazzaroni, R
    Berggren, Magnus
    Linköping University, The Institute of Technology. Linköping University, Department of Science and Technology.
    Salaneck, William R
    Linköping University, The Institute of Technology. Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry.
    Crispin, Xavier
    Linköping University, The Institute of Technology. Linköping University, Department of Science and Technology.
    Characterization of the interface dipole at the paraphenylenediamine-nickel interface: A joint theoretical and experimental study2005In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 122, no 8, p. 84712-Article in journal (Refereed)
    Abstract [en]

    In organic-based (opto)electronic devices, charge injection into conjugated materials is governed to a large extent by the metal-organic interface dipole. Controlling the injection of charges requires a better understanding of the fundamental origin of the interface dipole. In this context, photoelectron spectroscopies and density functional theory calculations are used to investigate the interaction between para-phenylenediamine (PPDA), an electron donor, and a polycrystalline nickel surface. The interface dipole formed upon chemisorption of one PPDA monolayer strongly modifies the work function of the nickel surface from 5.10 to 3.55 eV. The work function decrease of 1.55 eV is explained by the electron-donor character of PPDA and the modification of the electronic density at the metal surface. PPDA monolayers are composed of tilted molecules interacting via the nitrogen lone-pair and PPDA molecules chemisorbed parallel to the surface via their π-electron density. Annealing the monolayer leads to dehydrogenation of PPDA activated by the nickel surface, as found for other amines.

  • 103.
    Lindell, Linda
    et al.
    Linköping University, The Institute of Technology. Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry.
    Jakobsson, Fredrik
    Linköping University, The Institute of Technology. Linköping University, Department of Science and Technology.
    Osikowicz, Wojciech
    Linköping University, The Institute of Technology. Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry.
    Andersson, Peter
    Linköping University, The Institute of Technology. Linköping University, Department of Science and Technology.
    Salaneck, William R
    Linköping University, The Institute of Technology. Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry.
    Berggren, Magnus
    Linköping University, The Institute of Technology. Linköping University, Department of Science and Technology.
    Cornil, Jerome
    Crispin, Xavier
    Linköping University, The Institute of Technology. Linköping University, Department of Science and Technology.
    Towards Transparent Inorganic and Plastic Low-Workfunction Electrodes2005In: MRS Fall Meeting,2005, 2005Conference paper (Refereed)
  • 104.
    Lindell, Linda
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry . Linköping University, The Institute of Technology.
    Unge, Mikael
    Linköping University, Department of Physics, Chemistry and Biology, Computational Physics . Linköping University, The Institute of Technology.
    Osikowicz, Wojciech
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry . Linköping University, The Institute of Technology.
    Stafström, Sven
    Linköping University, Department of Physics, Chemistry and Biology, Computational Physics . Linköping University, The Institute of Technology.
    Salaneck, William R
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry . Linköping University, The Institute of Technology.
    Crispin, Xavier
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    de Jong, Michael P
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry . Linköping University, The Institute of Technology.
    Integer charge transfer at the tetrakis(dimethylamino)ethylene/Au interface2008In: Applied Physics Letters, ISSN 0003-6951, E-ISSN 1077-3118, Vol. 92, no 16, p. 163302-1-163302-3Article in journal (Refereed)
    Abstract [en]

    In organic-based electronics, interfacial properties have a profound impact on device performance. The lineup of energy levels is usually dependent on interface dipoles, which may arise from charge transfer reactions. In many applications, metal-organic junctions are prepared under ambient conditions, where direct overlap of the organic system from the metal bands is prevented due to presence of oxides and/or hydrocarbons. We present direct experimental and theoretical evidence showing that the interface energetic for such systems is governed by exchange of an integer amount of electrons.

  • 105.
    Liu, Jiang
    et al.
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Engquist, Isak
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Crispin, Xavier
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Spatial Control of p-n Junction in an Organic Light-Emitting Electrochemical Transistor2012In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 134, no 2, p. 901-904Article in journal (Refereed)
    Abstract [en]

    Low-voltage-operating organic electrochemical light-emitting cells (LECs) and transistors (OECTs) can be realized in robust device architectures, thus enabling easy manufacturing of light sources using printing tools. In an LEC, the p-n junction, located within the organic semiconductor channel, constitutes the active light-emitting element. It is established and fixated through electrochemical p- and n-doping, which are governed by charge injection from the anode and cathode, respectively. In an OECT, the electrochemical doping level along the organic semiconducting channel is controlled via the gate electrode. Here we report the merger of these two devices: the light-emitting electrochemical transistor, in which the location of the emitting p-n junction and the current level between the anode and cathode are modulated via a gate electrode. Light emission occurs at 4 V, and the emission zone can be repeatedly moved back and forth within an interelectrode gap of 500 mu m by application of a 4 V gate bias. In transistor operation, the estimated on/off ratio ranges from 10 to 100 with a gate threshold voltage of -2.3 V and transconductance value between 1.4 and 3 mu S. This device structure opens for new experiments tunable light sources and LECs with added electronic functionality.

  • 106.
    Liu, Jiang
    et al.
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Herlogsson, Lars
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Sawadtee, A
    Acreo AB.
    Favia, P
    IMEC.
    Sandberg, M
    Acreo AB.
    Crispin, Xavier
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Engquist, Isak
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Berggren, Magnus
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Vertical polyelectrolyte-gated organic field-effect transistors2010In: Applied Physics Letters, ISSN 0003-6951, E-ISSN 1077-3118, Vol. 97, p. 103303-Article in journal (Refereed)
    Abstract [en]

    Short-channel, vertically structured organic transistors with a polyelectrolyte as gate insulator are demonstrated. The devices are fabricated using low-resolution, self-aligned, and mask-free photolithography. Owing to the use of a polyelectrolyte, our vertical electrolyte-gated organic field-effect transistors (VEGOFETs), with channel lengths of 2.2 and 0.7 μm, operate at voltages below one volt. The VEGOFETs show clear saturation and switch on and off in 200 μs. A vertical geometry to achieve short-transistor channels and the use of an electrolyte makes these transistors promising candidates for printed logics and drivers with low operating voltage.

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  • 107.
    Malti, Abdellah
    et al.
    Linköping University, The Institute of Technology. Linköping University, Department of Science and Technology, Physics and Electronics.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Crispin, Xavier
    Linköping University, The Institute of Technology. Linköping University, Department of Science and Technology, Physics and Electronics.
    Low-voltage ambipolar polyelectrolyte-gated organic thin film transistors2012In: Applied Physics Letters, ISSN 0003-6951, E-ISSN 1077-3118, Vol. 100, no 18, p. 183302-Article in journal (Refereed)
    Abstract [en]

    Organic transistors that use polyelectrolytes as gate insulators can be driven at very low voltages (andlt;1 V). The low operating voltage is possible thanks to the formation of electric double layers upon polarization, which generates large electric fields at the critical interfaces in the device structure. In this work, we use a semiconducting blend (of a high electron affinity polymer and a low ionization potential one) in conjunction with a solid polyelectrolyte insulator to fabricate low-voltage ambipolar organic transistors. For both n- and p-channel operation, we use a polycation with readily mobile-yet large enough to limit bulk doping of the semiconductor-counterions.

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  • 108.
    Malti, Abdellah
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Brooke, Robert
    University of S Australia, Australia.
    Liu, Xianjie
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Zhao, Dan
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Andersson Ersman, Peter
    AcreoSwedish ICT, Sweden.
    Fahlman, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    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.
    A substrate-free electrochromic device2015Manuscript (preprint) (Other academic)
    Abstract [en]

    Electrochromic displays based on conducting polymers offer higher contrast, are cheaper, faster, more durable, and easier to synthesize as well as to process than their non-polymeric counterparts. The field of organic electrochromics has made considerable strides in the last decade with the development of new materials and methods. Here, we present a cellulose composite combining PEDOT:PSS and TiO2 that is a free-standing electrochromic material. Owing to the excellent refractive properties of TiO2, this nanocomposite is white in the neutral state and, when reduced, turns blue resulting in a color contrast exceeding 30. The composite has a granular morphology and, as shown by AFM, an intermingling of TiO2 and PEDOT:PSS at the surface. Variation of TiO2 within the material led to a trade-off in optical and electrical properties. A proof of concept free-standing electrochromic device was fabricated by casting several layers, which was found to be stable over 100 cycles.

  • 109.
    Malti, Abdellah
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Brooke, Robert
    Linköping University, Department of Science and Technology. 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.
    Zhao, Dan
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Andersson Ersman, Peter
    Acreo Swedish ICT, Sweden.
    Fahlman, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Jonsson, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    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.
    Freestanding electrochromic paper2016In: Journal of Materials Chemistry C, ISSN 2050-7526, E-ISSN 2050-7534, Vol. 4, no 41, p. 9680-9686Article in journal (Refereed)
    Abstract [en]

    Electrochromic displays based on conducting polymers exhibit higher contrasts and are cheaper, faster, more durable, and easier to synthesize as well as to process than their non-polymeric counterparts. However, current devices are typically based on thin electrochromic layers on top of a reflecting surface, which limits the thickness of the polymer layer to a few hundred nanometers. Here, we embed a light-scattering material within the electrochromic material to achieve a freestanding electrochromic paper-like electrode (50 to 500 mm). The device is based on a cellulose composite combining PEDOT:PSS as the electrochromic material and TiO2 nanoparticles as the reflecting material. Owing to the excellent refractive properties of TiO2, this nanocomposite is white in the neutral state and, when reduced, turns blue resulting in a color contrast around 30. The composite has a granular morphology and, as shown by AFM, an intermingling of TiO2 and PEDOT: PSS at the surface. Variation of the amount of TiO2 within the composite material is shown to result in a trade-off in optical and electrical properties. A proof-of-concept freestanding electrochromic device was fabricated by casting all layers successively to maximize the interlayer conformation. This freestanding device was found to be stable for over 100 cycles when ramped between 3 and -3 V.

  • 110.
    Malti, Abdellah
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Edberg, Jesper
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Granberg, Hjalmar
    Innventia AB, Stockholm, Sweden.
    Khan, Zia Ullah
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Andreasen, Jens W.
    Technical University of Denmark, Department of Energy Conversion and Storage, Roskilde, Denmark.
    Liu, Xianjie
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Zhao, Dan
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Zhang, Hao
    Department of Physics and Astronomy, University of Kentucky, Lexington, USA.
    Yao, Ylong
    Department of Physics and Astronomy, University of Kentucky, Lexington, USA.
    Brill, Joseph W.
    Department of Physics and Astronomy, University of Kentucky, Lexington, USA.
    Engquist, Isak
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Fahlman, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Wåberg, Lars
    KTH Royal Institute of Technology, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, and Wallenberg Wood Science Center, Stockholm, Sweden.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Enabling organic power electronics with a cellulose nano-scaffold2015Manuscript (preprint) (Other academic)
    Abstract [en]

    Exploiting the nanoscale properties of certain materials enables the creation of new materials with a unique set of properties. Here, we report on an electronic (and ionic) conducting paper based on cellulose nanofibrils (CNF) composited with poly(3,4-ethylene-dioxythiophene):poly(styrene-sulfonate) (PEDOT:PSS), which may be facilely processed into large three-dimensional geometries, while keeping unprecedented electronic and ionic conductivities of 140 S/cm and 20 mS/cm, respectively. This is achieved by cladding the CNF with PEDOT:PSS, and trapping an ion-transporting phase in the interstices between these nanofibrils. The unique properties of the resulting nanopaper composite have been used to demonstrate (electrochemical) transistors, supercapacitors and conductors resulting in exceptionally high device parameters, such as an associated transconductance, charge storage capacity and current level beyond 1 S, 1 F and 1 A, respectively.

  • 111.
    Malti, Abdellah
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Edberg, Jesper
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Granberg, Hjalmar
    Innventia AB, Stockholm.
    Ullah Khan, Zia
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Andreasen, Jens W
    Technical University of Denmark, Roskilde.
    Liu, Xianjie
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Zhao, Dan
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Zhang, Hao
    University of Kentucky, Lexington.
    Yao, Yulong
    University of Kentucky, Lexington.
    Brill, Joseph W
    University of Kentucky, Lexington.
    Engquist, Isak
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Fahlman, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Wågberg, Lars
    KTH Royal Institute of Technology, Stockholm.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    An Organic Mixed Ion–Electron Conductor for Power Electronics2016In: Advanced Science, ISSN 2198-3844, article id 1500305Article in journal (Refereed)
    Abstract [en]

    A mixed ionic–electronic conductor based on nanofibrillated cellulose composited with poly(3,4-ethylene-dioxythio­phene):­poly(styrene-sulfonate) along with high boiling point solvents is demonstrated in bulky electrochemical devices. The high electronic and ionic conductivities of the resulting nanopaper are exploited in devices which exhibit record values for the charge storage capacitance (1F) in supercapacitors and transconductance (1S) in electrochemical transistors.

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  • 112.
    Malti, Abdellah
    et al.
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Gabrielsson, Erik
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Crispin, Xavier
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Ultra-low voltage air-stable polyelectrolyte gated n-type organic thin film transistors2011In: Applied Physics Letters, ISSN 0003-6951, E-ISSN 1077-3118, Vol. 99, no 6, p. 063305-Article in journal (Refereed)
    Abstract [en]

    Complementary circuits, processing digital signals, are a cornerstone of modern electronics. Such circuits require both p-and n-type transistors. Polyelectrolytes are used as gate insulators in organic thin film transistors (OTFTs) to establish an electric double layer capacitor upon gate bias that allows low operational voltages (andlt;1 V). However, stable and low-voltage operating n-channel organic transistors have proven difficult to construct. Here, we report ultra-low voltage n-channel organic polymer-based transistors that are stable in ambient atmosphere. Our n-type OTFTs exhibit on/off ratios around 10(3) for an applied drain potential as low as 0.1 V. Since small ions are known to promote electrochemical reactions within the semiconductors channel bulk and typically slow down the transistor, we use a solid polycationic gate insulator that suppresses penetration of anions into the n-channel semiconductor. As a result, our n-channel OTFTs switch on in under 5 ms and off in less than 1 ms.

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  • 113.
    Malti, Abdellah
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Gabrielsson, Erik
    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.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    An Electrochromic Bipolar Membrane Diode2015In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 27, no 26, p. 3909-+Article in journal (Refereed)
    Abstract [en]

    Conducting polymers with bipolar membranes (a complementary stack of selective membranes) may be used to rectify current. Integrating a bipolar membrane into a polymer electrochromic display obviates the need for an addressing backplane while increasing the devices bistability. Such devices can be made from solution-processable materials.

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  • 114.
    Marciniak Braun, Slawomir
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, The Institute of Technology.
    Crispin, Xavier
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, The Institute of Technology.
    Uvdal, Kajsa
    Linköping University, Department of Physics, Chemistry and Biology, Sensor Science and Molecular Physics. Linköping University, The Institute of Technology.
    Trzcinski, M.
    Institute of Mathematics and Physics, Bydgoszcz, Poland.
    Birgerson, J.
    LCD Technology, Dalarna University, Borlänge, Sweden.
    Groenendaal, L.
    Agfa-Gevaert N. V., R&D Materials/Chemistry Department, Mortsel, Belgium.
    Louwet, F.
    Agfa-Gevaert N. V., R&D Materials/Chemistry Department, Mortsel, Belgium.
    Salaneck, William R.
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, The Institute of Technology.
    Light Induced Damage in Poly(3,4-ethylenedioxythiophene) and its Derivatives Studied by Photoelectron Spectroscopy2004In: Synthetic metals, ISSN 0379-6779, E-ISSN 1879-3290, Vol. 141, no 1-2, p. 67-73Article in journal (Refereed)
    Abstract [en]

    Poly(3,4-ethylenedioxythiophene), usually known as PEDOT, and derivatives have attracted significant interest because of their high electrical conductivity. This electric property, however, deteriorates upon exposure to solar radiation. X-ray photoelectron spectroscopy (XPS) has been used to study the UV-light-induced chemical changes in doped PEDOT, as well as in both neutral and doped forms of its alkylated derivative—PEDOT-C14H29. Analysis of the XPS data indicates an oxidation of the sulfur in the thiophene ring. Apparently, photo-oxidation leads to the formation of sulfon groups, SO2, resulting in a disruption of π-conjugation in PEDOT, which there by diminishes the conductivity of the organic layer. This hypothesis is supported by the results of a study of model molecules for pristine and the oxidized PEDOT unit: 3,4 ethylenedioxythiophene (EDOT) and 3,4 ethylenedioxythiophene and S-dioxide (EDOT-SO2), respectively.

  • 115.
    Mirsakiyeva, Amina
    et al.
    KTH Royal Institute Technology, Sweden.
    Hugosson, Håkan W.
    KTH Royal Institute Technology, Sweden; University of Gavle, Sweden.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Delin, Anna
    KTH Royal Institute Technology, Sweden; Uppsala University, Sweden.
    Quantum Molecular Dynamical Calculations of PEDOT 12-Oligomer and its Selenium and Tellurium Derivatives2017In: Journal of Electronic Materials, ISSN 0361-5235, E-ISSN 1543-186X, Vol. 46, no 5, p. 3071-3075Article in journal (Refereed)
    Abstract [en]

    We present simulation results, computed with the Car-Parrinello molecular dynamics method, at zero and ambient temperature (300 K) for poly(3,4-ethylenedioxythiophene) [PEDOT] and its selenium and tellurium derivatives PEDOS and PEDOTe, represented as 12-oligomer chains. In particular, we focus on structural parameters such as the dihedral rotation angle distribution, as well as how the charge distribution is affected by temperature. We find that for PEDOT, the dihedral angle distribution shows two distinct local maxima whereas for PEDOS and PEDOTe, the distributions only have one clear maximum. The twisting stiffness at ambient temperature appears to be larger the lighter the heteroatom (S, Se, Te) is, in contrast to the case at 0 K. As regards point charge distributions, they suggest that aromaticity increases with temperature, and also that aromaticity becomes more pronounced the lighter the heteroatom is, both at 0 K and ambient temperature. Our results agree well with previous results, where available. The bond lengths are consistent with substantial aromatic character both at 0 K and at ambient temperature. Our calculations also reproduce the expected trend of diminishing gap between the highest occupied molecular orbital and the lowest unoccupied molecular orbital with increasing atomic number of the heteroatom.

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  • 116.
    Mitraka, Evangelia
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Gryszel, Maciej
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Jafari, Mohammad Javad
    Linköping University, Department of Physics, Chemistry and Biology, Molecular Physics. Linköping University, Faculty of Science & Engineering.
    Singh, Amritpal
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Warczak, Magdalena
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Mitrakas, Manassis
    Aristotle University of Thessaloniki, Thessaloniki, Greece.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Ederth, Thomas
    Linköping University, Department of Physics, Chemistry and Biology, Molecular Physics. Linköping University, Faculty of Science & Engineering.
    Zozoulenko, Igor
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Glowacki, Eric
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Electrocatalytic Production of Hydrogen Peroxide with Poly(3,4-ethylenedioxythiophene) Electrodes2019In: Advanced Sustainable Systems, ISSN 2366-7486, Vol. 3, no 2, p. 1-6, article id 1800110Article in journal (Refereed)
    Abstract [en]

    Electrocatalysis for energy‐efficient chemical transformations is a central concept behind sustainable technologies. Numerous efforts focus on synthesizing hydrogen peroxide, a major industrial chemical and potential fuel, using simple and green methods. Electrochemical synthesis of peroxide is a promising route. Herein it is demonstrated that the conducting polymer poly(3,4‐ethylenedioxythiophene), PEDOT, is an efficient and selective heterogeneous catalyst for the direct reduction of oxygen to hydrogen peroxide. While many metallic catalysts are known to generate peroxide, they subsequently catalyze decomposition of peroxide to water. PEDOT electrodes can support continuous generation of high concentrations of peroxide with Faraday efficiency remaining close to 100%. The mechanisms of PEDOT‐catalyzed reduction of O2 to H2O2 using in situ spectroscopic techniques and theoretical calculations, which both corroborate the existence of a chemisorbed reactive intermediate on the polymer chains that kinetically favors the selective reduction reaction to H2O2, are explored. These results offer a viable method for peroxide electrosynthesis and open new possibilities for intrinsic catalytic properties of conducting polymers.

  • 117.
    Mitraka, Evangelia
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Jafari, Mohammad Javad
    Linköping University, Department of Physics, Chemistry and Biology, Molecular Physics. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. 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.
    Fahlman, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Ederth, Thomas
    Linköping University, Department of Physics, Chemistry and Biology, Molecular Physics. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Jonsson, Magnus
    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.
    Oxygen-induced doping on reduced PEDOT2017In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 5, no 9, p. 4404-4412Article in journal (Refereed)
    Abstract [en]

    The conducting polymer poly(3,4-ethylenedioxythiophene) (PEDOT) has shown promise as air electrode in renewable energy technologies like metal-air batteries and fuel cells. PEDOT is based on atomic elements of high abundance and is synthesized at low temperature from solution. The mechanism of oxygen reduction reaction (ORR) over chemically polymerized PEDOT: Cl still remains controversial with eventual role of transition metal impurities. However, regardless of the mechanistic route, we here demonstrate yet another key active role of PEDOT in the ORR mechanism. Our study demonstrates the decoupling of conductivity (intrinsic property) from electrocatalysis (as an extrinsic phenomenon) yielding the evidence of doping of the polymer by oxygen during ORR. Hence, the PEDOT electrode is electrochemically reduced (undoped) in the voltage range of ORR regime, but O-2 keeps it conducting; ensuring PEDOT to act as an electrode for the ORR. The interaction of oxygen with the polymer electrode is investigated with a battery of spectroscopic techniques.

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  • 118.
    Mitraka, Evangelia
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Kergoat, Loig
    Linköping University, Department of Science and Technology. 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.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Douheret, O.
    University of Mons UMons, Belgium.
    Leclere, P.
    University of Mons UMons, Belgium.
    Nilsson, M.
    Acreo AB, Sweden.
    Andersson Ersman, P.
    Acreo AB, Sweden.
    Gustafsson, G.
    Acreo AB, Sweden.
    Lazzaroni, R.
    University of Mons UMons, Belgium.
    Berggren, Magnus
    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.
    Solution processed liquid metal-conducting polymer hybrid thin films as electrochemical pH-threshold indicators2015In: Journal of Materials Chemistry C, ISSN 2050-7526, E-ISSN 2050-7534, Vol. 3, no 29, p. 7604-7611Article in journal (Refereed)
    Abstract [en]

    A global and accurate mapping of the environment could be achieved if sensors and indicators are mass-produced at low cost. Printed electronics using polymeric (semi) conductors offer a platform for such sensor/indicator based circuits. Herein, we present the material concept for an electrochemical pH-threshold indicator based on a printable hybrid electrode which comprises a liquid metal alloy (GaInSn) embedded in a conducting polymer matrix (PEDOT). This hybrid electrode displays a large variation in open circuit potential versus pH in an electrochemical cell, which when connected to the gate of an electrochemical transistor leads to a dramatic change in the drain current in a narrow range of pH.

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  • 119.
    Mitraka, Evangelia
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Sjoestedt, Anna
    RISE Bioecon, Sweden.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Hakansson, Karl M. O.
    RISE Bioecon, Sweden.
    Jonsson, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    PEDOT-Cellulose Gas Diffusion Electrodes for Disposable Fuel CellsIn: ADVANCED SUSTAINABLE SYSTEMS, ISSN 2366-7486, article id 1900097Article in journal (Refereed)
    Abstract [en]

    The mass implementation of renewable energy sources is limited by the lack of energy storage solutions operating on various timescales. Electrochemical technologies such as supercapacitors and batteries cannot handle long storage time because of self-discharge issues. The combination of fuel storage technology and fuel cells is an attractive solution for long storage times. In that context, large-scale fuel cell solutions are required for massive energy storage in cities, which leads to possible concepts such as low-cost disposable fully organic membrane assemblies in fuel cells to avoid regeneration of expensive poisoned electrodes. Here, the formation of an organic gas diffusion electrode (GDE) fabricated by paper-making production, combined with in situ polymerization is demonstrated for the first time. Cellulose is used as a 3D scaffold functionalized with poly(3,4-ethylenedioxythiophene) (PEDOT) serving as both an electrical conductor and an electrocatalyst of high efficiency for the oxygen reduction reaction. The PEDOT-cellulose porous GDE is implemented in a membrane assembly and demonstrated in a H-2-O-2 fuel cell. The demonstration of low-cost material/manufacturing that is environmentally friendly is a paradigm shift in the development of fuel cells for a sustainable society.

  • 120.
    Munoz, William Armando
    et al.
    Linköping University, Department of Science and Technology. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Fahlman, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Zozoulenko, Igor
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Understanding the Impact of Film Disorder and Local Surface Potential in Ultraviolet Photoelectron Spectroscopy of PEDOT2018In: Macromolecular rapid communications, ISSN 1022-1336, E-ISSN 1521-3927, Vol. 39, no 4, article id 1700533Article in journal (Refereed)
    Abstract [en]

    The spectra of conducting polymers obtained using ultraviolet photoelectron spectroscopy (UPS) exhibit a typical broadening of the tail sigma(UPS) approximate to 1 eV, which by an order of magnitude exceeds a commonly accepted value of the broadening of the tail of the density of states sigma(DOS) approximate to 0.1 eV obtained using transport measurements. In this work, an origin of this anomalous broadening of the tail of the UPS spectra in a doped conducting polymer, PEDOT (poly(3,4-ethylenedioxythiophene)), is discussed. Based on the semiempirical approach and using a realistic morphological model, the density of valence states in PEDOT doped with molecular counterions is computed. It is shown that due to a disordered character of the material with randomly distributed counterions, the localized charge carriers in PEDOT crystallites experience spatially varying electrostatic potential. This leads to spatially varying local vacuum levels and binding energies. Taking this variation into account the UPS spectrum is obtained with the broadening of the tail comparable to the experimentally observed one. The results imply that the observed broadening of the tail of the UPS spectra in PEDOT provides information about a disordered spatially varying potential in the material rather than the broadening of the DOS itself.

  • 121.
    Munoz, William Armando
    et al.
    Linköping University, Department of Science and Technology. Linköping University, Faculty of Science & Engineering.
    Singh, Sandeep Kumar
    Linköping University, Department of Science and Technology. Linköping University, Faculty of Science & Engineering.
    Franco Gonzalez, Felipe
    Linköping University, Department of Science and Technology. Linköping University, Faculty of Science & Engineering.
    Linares, Mathieu
    Linköping University, Department of Physics, Chemistry and Biology, Bioinformatics. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Zozoulenko, Igor
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Insulator to semimetallic transition in conducting polymers2016In: Physical Review B, ISSN 2469-9950, E-ISSN 2469-9969, Vol. 94, no 20, article id 205202Article in journal (Refereed)
    Abstract [en]

    We report a multiscale modeling of electronic structure of a conducting polymer poly(3,4-ethylenedioxythiopehene) (PEDOT) based on a realistic model of its morphology. We show that when the charge carrier concentration increases, the character of the density of states (DOS) gradually evolves from the insulating to the semimetallic, exhibiting a collapse of the gap between the bipolaron and valence bands with the drastic increase of the DOS between the bands. The origin of the observed behavior is attributed to the effect of randomly located counterions giving rise to the states in the gap. These results are discussed in light of recent experiments. The method developed in this work is general and can be applied to study the electronic structure of other conducting polymers.

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  • 122.
    Méhes, Gábor
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Mulla, Yusuf
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Granberg, Hjalmar
    Res Inst Sweden, Sweden.
    Che, Canyan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Beni, Valerio
    Res Inst Sweden, Sweden.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Stavrinidou, Eleni
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Simon, Daniel
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Solar Heat-Enhanced Energy Conversion in Devices Based on Photosynthetic Membranes and PEDOT:PSS-Nanocellulose Electrodes2020In: ADVANCED SUSTAINABLE SYSTEMS, ISSN 2366-7486, article id 1900100Article in journal (Refereed)
    Abstract [en]

    Energy harvesting from photosynthetic membranes, proteins, or bacteria through bio-photovoltaic or bio-electrochemical approaches has been proposed as a new route to clean energy. A major shortcoming of these and solar cell technologies is the underutilization of solar irradiation wavelengths in the IR region, especially those in the far IR region. Here, a biohybrid energy-harvesting device is demonstrated that exploits IR radiation, via convection and thermoelectric effects, to improve the resulting energy conversion performance. A composite of nanocellulose and the conducting polymer system poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) is used as the anode in biohybrid cells that includes thylakoid membranes (TMs) and redox mediators (RMs) in solution. By irradiating the conducting polymer electrode by an IR light-emitting diode, a sixfold enhancement in the harvested bio-photovoltaic power is achieved, without compromising stability of operation. Investigation of the output currents reveals that IR irradiation generates convective heat transfer in the electrolyte bulk, which enhances the redox reactions of RMs at the anode by suppressing diffusion limitations. In addition, a fast-transient thermoelectric component, originating from the PEDOT:PSS-nanocellulose-electrolyte interphase, further increases the bio-photocurrent. These results pave the way for the development of energy-harvesting biohybrids that make use of heat, via IR absorption, to enhance energy conversion efficiency.

  • 123.
    Osikowicz, Wojciech
    et al.
    Linköping University, The Institute of Technology. Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry .
    Crispin, Xavier
    Linköping University, The Institute of Technology. Linköping University, Department of Science and Technology.
    Tengstedt, Carl
    Linköping University, The Institute of Technology. Linköping University, Department of Science and Technology.
    Lindell, Linda
    Linköping University, The Institute of Technology. Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry .
    Kugler, Thomas
    Linköping University, The Institute of Technology. Linköping University, Department of Science and Technology.
    Salaneck, William R
    Linköping University, The Institute of Technology. Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry .
    Transparent low-work-function indium tin oxide electrode obtained by molecular scale interface engineering2004In: Applied Physics Letters, ISSN 0003-6951, E-ISSN 1077-3118, Vol. 85, no 9, p. 1616-1618Article in journal (Refereed)
    Abstract [en]

    Transparent low-work-function indium tin oxide (ITO) electrode was obtained by using molecular scale interface engineering. The modified ITO surface may be used as electron injecting electrode in polymer light-emitting devices. ITO surfaces, exposed to TDAE molecules, were found to be stable upon exposure to air, and to mild annealing. Photoelectron spectroscopy measurements show that the low-work-function of the modified electrode remains upon exposure to air in gentle annealing.

  • 124.
    Osikowicz, Wojciech
    et al.
    Linköping University, The Institute of Technology. Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry .
    Van, Der Gon A.W.D.
    Van Der Gon, A.W.D., Department of Applied Physics, Eindhoven Univ. of Technology, PO Box 513, 5600 MB Eindhoven, Netherlands.
    Crispin, Xavier
    Linköping University, The Institute of Technology. Linköping University, Department of Science and Technology.
    de Jong, Michel P
    Linköping University, The Institute of Technology. Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry .
    Friedlein, Rainer
    Linköping University, The Institute of Technology. Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry .
    Groenendaal, L.
    AGFA-Gevaert N.V., R and D Mat. - Chem. Dept., Septestraat 27, B-2640 Mortsel, Belgium.
    Fahlman, Mats
    Linköping University, The Institute of Technology. Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry .
    Beljonne, D.
    Serv. Chim. des Materiaux Nouveaux, CREPM, Université de Mons-Hainaut, Place du Parc 20, B-7000 Mons, Belgium.
    Lazzaroni, R.
    Serv. Chim. des Materiaux Nouveaux, CREPM, Université de Mons-Hainaut, Place du Parc 20, B-7000 Mons, Belgium.
    Salaneck, William R
    Linköping University, The Institute of Technology. Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry .
    A joint theoretical and experimental study on the electronic properties of phenyl-capped 3,4-ethylenedioxythiophene oligomers2003In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 119, no 19, p. 10415-10420Article in journal (Refereed)
    Abstract [en]

    The electronic structure of a series of phenyl-capped EDOT oligomers was studied using ultraviolet photoelectron spectroscopy, in combination with quantum-chemical methods. The bulk IP of the neutral PEDOT polymer was estimated to be 4.2 eV. The frontier band structue was predicted from the evolution of the spectral features in the studied series of oligomers.

  • 125.
    Petsagkourakis, Ioannis
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Kim, Nara
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Tybrandt, Klas
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Zozoulenko, Igor
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Poly(3,4-ethylenedioxythiophene): Chemical Synthesis, Transport Properties, and Thermoelectric Devices2019In: ADVANCED ELECTRONIC MATERIALS, ISSN 2199-160X, Vol. 5, no 11Article, review/survey (Refereed)
    Abstract [en]

    Since their discovery in the seventies, conducting polymers have been chemically designed to acquire specific optical and electrical properties for various applications. Poly(3,4-ethylenedioxythiophene) (PEDOT) is among the most successful polymers as indicated by approximate to 12 000 articles mentioning it to date. PEDOT is found as transparent polymer electrodes in solar cells and light-emitting diodes, as printed electrodes in transistors, and as the main component of electrochromic displays, supercapacitors, and electrochemical transistors. For around seven years, PEDOT has been classified as the first thermoelectric polymer that converts heat flow into electricity. This has triggered a renewed interest in the scientific community, with about 400 publications including the keyword "PEDOT" and "thermoelectric." Among the topics covered by those scientific works are: i) the optimization of the thermoelectric properties, ii) understanding of the interplay between electrical properties and morphology, iii) the origin of the Seebeck coefficient, iv) the characterization of its thermal conductivity; and v) the design of thermoelectric devices. This work aims to be a pedagogical introduction to PEDOT but also to review the state-of-the art of its thermoelectric properties and thermoelectric devices. Hopefully, this work will inspire scientists to find chemical design rules to bring organic thermoelectrics beyond PEDOT.

  • 126.
    Petsagkourakis, Ioannis
    et al.
    University of Bordeaux, France.
    Pavlopoulou, Eleni
    Institute Polytech Bordeaux Bordeaux INP, France.
    Cloutet, Eric
    University of Bordeaux, France.
    Fang Chen, Yan
    University of Bordeaux, France.
    Liu, Xianjie
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Fahlman, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    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.
    Dilhaire, Stefan
    University of Bordeaux, France.
    Fleury, Guillaume
    University of Bordeaux, France.
    Hadziioannou, Georges
    University of Bordeaux, France.
    Correlating the Seebeck coefficient of thermoelectric polymer thin films to their charge transport mechanism2018In: Organic electronics, ISSN 1566-1199, E-ISSN 1878-5530, Vol. 52, p. 335-341Article in journal (Refereed)
    Abstract [en]

    Room temperature flexible heat harvesters based on conducting polymers are ideally suited to cover the energy demands of the modern nomadic society. The optimization of their thermoelectric efficiency is usually sought by tuning the oxidation levels of the conducting polymers, even if such methodology is detrimental to the Seebeck coefficient (S) as both the Seebeck coefficient and the electrical conductivity (sigma) are antagonistically related to the carrier concentration. Here we report a concurrent increase of S and sigma and we experimentally derive the dependence of Seebeck coefficient on charge carrier mobility for the first time in organic electronics. Through specific control of the conducting polymer synthesis, we enabled the formation of a denser percolation network that facilitated the charge transport and the thermodiffusion of the charge carriers inside the conducting polymer layer, while the material shifted from a Fermi glass towards a semi-metal, as its crystallinity increased. This work sheds light upon the origin of the thermoelectric properties of conducting polymers, but also underlines the importance of enhanced charge carrier mobility for the design of efficient thermoelectric polymers.

  • 127.
    Petsagkourakis, Ioannis
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Tybrandt, Klas
    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.
    Ohkubo, Isao
    Natl Inst Mat Sci, Japan.
    Satoh, Norifusa
    Natl Inst Mat Sci, Japan.
    Mori, Takao
    Natl Inst Mat Sci, Japan; Univ Tsukuba, Japan.
    Thermoelectric materials and applications for energy harvesting power generation2018In: Science and Technology of Advanced Materials, ISSN 1468-6996, E-ISSN 1878-5514, Vol. 19, no 1, p. 836-862Article, review/survey (Refereed)
    Abstract [en]

    Thermoelectrics, in particular solid-state conversion of heat to electricity, is expected to be a key energy harvesting technology to power ubiquitous sensors and wearable devices in the future. A comprehensive review is given on the principles and advances in the development of thermoelectric materials suitable for energy harvesting power generation, ranging from organic and hybrid organic-inorganic to inorganic materials. Examples of design and applications are also presented. [GRAPHICS] .

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  • 128.
    Rudd, Sam
    et al.
    University of South Australia, Australia.
    Franco Gonzalez, Felipe
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Singh, Sandeep Kumar
    Linköping University, Department of Science and Technology. 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.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Andreasen, Jens W.
    Technical University of Denmark, Denmark.
    Zozoulenko, Igor
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Evans, Drew
    University of South Australia, Australia.
    Charge transport and structure in semimetallic polymers2018In: Journal of Polymer Science Part B: Polymer Physics, ISSN 0887-6266, E-ISSN 1099-0488, Vol. 56, no 1, p. 97-104Article in journal (Refereed)
    Abstract [en]

    Owing to changes in their chemistry and structure, polymers can be fabricated to demonstrate vastly different electrical conductivities over many orders of magnitude. At the high end of conductivity is the class of conducting polymers, which are ideal candidates for many applications in low-cost electronics. Here, we report the influence of the nature of the doping anion at high doping levels within the semi-metallic conducting polymer poly(3,4-ethylenedioxythiophene) (PEDOT) on its electronic transport properties. Hall effect measurements on a variety of PEDOT samples show that the choice of doping anion can lead to an order of magnitude enhancement in the charge carrier mobilityamp;gt;3 cm(2)/Vs at conductivities approaching 3000 S/cm under ambient conditions. Grazing Incidence Wide Angle X-ray Scattering, Density Functional Theory calculations, and Molecular Dynamics simulations indicate that the chosen doping anion modifies the way PEDOT chains stack together. This link between structure and specific anion doping at high doping levels has ramifications for the fabrication of conducting polymer-based devices. (c) 2017 The Authors. Journal of Polymer Science Part B: Polymer Physics Published by Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2018, 56, 97-104

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  • 129.
    Said, Elias
    et al.
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Andersson, Peter
    ACREO AB, Bredgatan 34, SE-602 21 Norrköping, Sweden.
    Engquist, Isak
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Crispin, Xavier
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Berggren, Magnus
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Electrochromic display cells driven by an electrolyte-gated organic field-effect transistor2009In: Organic electronics, ISSN 1566-1199, E-ISSN 1878-5530, Vol. 10, no 6, p. 1195-1199Article in journal (Refereed)
    Abstract [en]

    Monolithic integration of an electrolyte-gated organic field-effect transistor (OFET) and an organic electrochromic pixel is reported. Thanks to its versatility, the polyanionic proton conductor poly(styrenesulfonic acid) (PSSH) can serve both as the gate “insulator” in OFETs and as the electrolyte in electrochromic display pixels. Employing identical materials in both the display cells and in the driver transistors is a necessary prerequisite to achieve robust displays possible to manufacture on flexible carriers using printing tools. Smart pixels combining depletion mode electrochemical transistors and electrochromic displays have been reported in the past. Here, an enhancement mode OFET as the driver enables relatively shorter updating times and much simpler addressing and updating schemes.

  • 130.
    Said, Elias
    et al.
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Crispin, Xavier
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Herlogsson, Lars
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Elhag, Sami
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Robinson, Nathaniel D.
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Berggren, Magnus
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Polymer field-effect transistor gated via a poly(styrenesulfonic acid) thin film2006In: Applied Physics Letters, ISSN 0003-6951, E-ISSN 1077-3118, Vol. 89, no 14, p. 143507-Article in journal (Refereed)
    Abstract [en]

    A polyanionic proton conductor, named poly(styrenesulfonic acid) (PSSH), is used to gate an organic field-effect transistor (OFET) based on poly(3-hexylthiophene) (P3HT). Upon applying a gate bias, large electric double layer capacitors (EDLCs) are formed quickly at the gate-PSSH and P3HT-PSSH interfaces due to proton migration in the polyelectrolyte. This type of robust transistor, called an EDLC-OFET, displays fast response (<1  ms) and operates at low voltages (<1  V). The results presented are relevant for low-cost printed polymer electronics.

  • 131.
    Said, Elias
    et al.
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Larsson, Oscar
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Berggren, Magnus
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Crispin, Xavier
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Effects of the Ioinc Currents in Electrolyte-gated Organic Field-Effect Transistors2008In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 18, no 21, p. 3529-3536Article in journal (Refereed)
    Abstract [en]

    Polyelectrolytes are promising materials as gate dielectrics in organic field-effect transistors (OFETs). Upon gate bias, their polarization induces an ionic charging current, which generates a large double layer capacitor (10-500 µF cm-2) at the semiconductor/electrolyte interface. The resulting transistor operates at low voltages (<1 V) and its conducting channel is formed in 50 µs. The effect of ionic currents on the performance of the OFETs is investigated by varying the relative humidity of the device ambience. Within defined humidity levels and potential values, the water electrolysis is negligible and the OFETs performances are optimum.

  • 132.
    Said, Elias
    et al.
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Larsson, Oscar
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Berggren, Magnus
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Crispin, Xavier
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Role of the ionic currents in electrolyte-gated organic field effect transistorsManuscript (Other (popular science, discussion, etc.))
  • 133.
    Shiran Chaharsoughi, Mina
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Zhao, Dan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Jonsson, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Thermodiffusion-Assisted Pyroelectrics-Enabling Rapid and Stable Heat and Radiation Sensing2019In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 29, no 28, article id 1900572Article in journal (Refereed)
    Abstract [en]

    Sensors for monitoring temperature, heat flux, and thermal radiation are essential for applications such as electronic skin. While pyroelectric and thermoelectric effects are suitable candidates as functional elements in such devices, both concepts show individual drawbacks in terms of zero equilibrium signals for pyroelectric materials and small or slow response of thermoelectric materials. Here, these drawbacks are overcome by introducing the concept of thermodiffusion-assisted pyroelectrics, which combines and enhances the performance of pyroelectric and ionic thermoelectric materials. The presented integrated concept provides both rapid initial response upon heating and stable synergistically enhanced signals upon prolonged exposure to heat stimuli. Likewise, incorporation of plasmonic metasurfaces enables the concept to provide both rapid and stable signals for radiation-induced heating. The performance of the concept and its working mechanism can be explained by ion-electron interactions at the interface between the pyroelectric and ionic thermoelectric materials.

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  • 134.
    Singh, Sandeep Kumar
    et al.
    Linköping University, Department of Science and Technology. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Zozoulenko, Igor
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Oxygen Reduction Reaction in Conducting Polymer PEDOT: Density Functional Theory Study2017In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 121, no 22, p. 12270-12277Article in journal (Refereed)
    Abstract [en]

    An oxygen reduction reaction (ORR) mechanism in conducting polymer PEDOT is studied using the density functional theory. It is demonstrated that pure PEDOT chains possess the catalytic activity, where no platinum catalyst or external dopants are needed to sustain the electrocatalysis. This remarkable property of PEDOT is related to the formation of polaronic states, which leads to the decrease of the HOMO LUMO gap and thus to the enhancement of the reactivity of the system. It is shown that ORR on PEDOT chains can proceed via two pathways, whether via a four-electron process when the oxygen reacts with protons and is reduced directly into water in four steps (Reaction path I) or via the two-electron process leading to formation of the hydrogen peroxide as an intermediate specimen (Reaction path II). Path I is demonstrated to be energetically preferable. This conclusion also holds for ORR on two pi-pi stacked chains and ORR for the case when PEDOT is reduced during the reaction. It is also found that ORR on PEDOT effectively proceeds in the presence of H3O+ but does not occur in the absence of acidic environment.

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  • 135.
    Sinno, Hiam
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Engquist, Isak
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Bias stress effect in polyelectrolyte-gated organic field-effect transistors2013In: Applied Physics Letters, ISSN 0003-6951, E-ISSN 1077-3118, Vol. 102, no 11Article in journal (Refereed)
    Abstract [en]

    A main factor contributing to bias stress instability in organic transistors is charge trapping of mobile carriers near the gate insulator-semiconductor interface into localized electronic states. In this paper, we study the bias stress behavior in low-voltage (p-type) polyelectrolyte-gated organic field effect transistors (EGOFETs) at various temperatures. Stressing and recovery in these EGOFETs are found to occur six orders of magntiude faster than typical bias stress/recovery reported for dielectric-gated OFETs. The mechanism proposed for EGOFETs involves an electron transfer reaction between water and the charged semiconductor channel that promotes the creation of extra protons diffusing into the polyelectrolyte.

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  • 136.
    Sinno, Hiam
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Kergoat, Loig
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Fabiano, Simone
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Engquist, Isak
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Bias stress effect in inverters based on polyelectrolyte-gated organic field effect transistors2013Manuscript (preprint) (Other academic)
    Abstract [en]

    Prolonged gate bias application causes undesirable operational instabilities in organic transistors involving threshold voltage shift and drain current degradation; an effect known as bias stress. In this paper, we report how this instability is manifested in inverter circuits based on polyelectrolytegated p-type organic field effect transistors (EGOFETs) operating at low voltage. We find that bias stress causes a significant, but recoverable, shift in inverter switching threshold voltage. Measurements with two different polyelectrolytes reveal significant differences in the stressing and recovery behaviour, which is ascribed to the distinct nature of the ion conductive groups in the polyelectrolyte. Moreover, we report a large influence of illumination on the recovery process for one of the polyelectrolytes but not for the other, which demonstrates the need to characterize bias stress behavior for each new materials combination.

  • 137.
    Sinno, Hiam
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Nguyen, Ha Tran
    University of Mons-UMONS, Belgium.
    Hägerström, Anders
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Fahlman, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, The Institute of Technology.
    Lindell, Linda
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, The Institute of Technology.
    Coulembier, Olivier
    University of Mons-UMONS, Belgium.
    Dubois, Philippe
    University of Mons-UMONS, Belgium.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Engquist, Isak
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Amphiphilic semiconducting copolymer as compatibility layer for printing polyelectrolyte-gated OFETs2013In: Organic electronics, ISSN 1566-1199, E-ISSN 1878-5530, Vol. 14, no 3, p. 790-796Article in journal (Refereed)
    Abstract [en]

    We report a method for inkjet-printing an organic semiconductor layer on top of the electrolyte insulator layer in polyelectrolyte-gated OFETs by using a surface modification treatment to overcome the underlying wettability problem at this interface. The method includes depositing an amphiphilic diblock copolymer (P3HT-b-PDMAEMA). This material is designed to have one set of blocks that mimics the hydrophobic properties of the semiconductor (poly(3-hexylthiophene) or P3HT), while the other set of blocks include polar components that improve adhesion to the polyelectrolyte insulator. Contact angle measurements, atomic force microscopy, and X-ray photoelectron spectroscopy confirm formation of the desired surface modification film. Successful inkjet printing of a smooth semiconductor layer allows us to manufacture complete transistor structures that exhibit low-voltage operation in the range of 1 V.

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  • 138.
    Stavrinidou, Eleni
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Gabrielsson, Roger
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Gomez, Eliot
    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.
    Nilsson, Ove
    Department of Forest Genetics and Plant Physiology, Swedish University of Agricultural Sciences, SE-901 87 Umeå, Sweden..
    Simon, Daniel T.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Electronic plants2015In: Science Advances, ISSN 2375-2548, Vol. 1, no 10, p. 1-8, article id e1501136Article in journal (Refereed)
    Abstract [en]

    The roots, stems, leaves, and vascular circuitry of higher plants are responsible for conveying the chemical signals that regulate growth and functions. From a certain perspective, these features are analogous to the contacts, interconnections, devices, and wires of discrete and integrated electronic circuits. Although many attempts have been made to augment plant function with electroactive materials, plants’ “circuitry” has never been directlymerged with electronics. We report analog and digital organic electronic circuits and devices manufactured in living plants. The four key components of a circuit have been achieved using the xylem, leaves, veins, and signals of the plant as the template and integral part of the circuit elements and functions. With integrated and distributed electronics in plants, one can envisage a range of applications including precision recording and regulation of physiology, energy harvesting from photosynthesis, and alternatives to genetic modification for plant optimization.

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  • 139.
    Sun, Hengda
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    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.
    Wang, Suhao
    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.
    Forchheimer, Robert
    Linköping University, Department of Electrical Engineering, Information Coding. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Complementary Logic Circuits Based on High-Performance n-Type Organic Electrochemical Transistors2018In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 30, no 9, article id 1704916Article in journal (Refereed)
    Abstract [en]

    Organic electrochemical transistors (OECTs) have been the subject of intense research in recent years. To date, however, most of the reported OECTs rely entirely on p-type (hole transport) operation, while electron transporting (n-type) OECTs are rare. The combination of efficient and stable p-type and n-type OECTs would allow for the development of complementary circuits, dramatically advancing the sophistication of OECT-based technologies. Poor stability in air and aqueous electrolyte media, low electron mobility, and/or a lack of electrochemical reversibility, of available high-electron affinity conjugated polymers, has made the development of n-type OECTs troublesome. Here, it is shown that ladder-type polymers such as poly(benzimidazobenzophenanthroline) (BBL) can successfully work as stable and efficient n-channel material for OECTs. These devices can be easily fabricated by means of facile spray-coating techniques. BBL-based OECTs show high transconductance (up to 9.7 mS) and excellent stability in ambient and aqueous media. It is demonstrated that BBL-based n-type OECTs can be successfully integrated with p-type OECTs to form electrochemical complementary inverters. The latter show high gains and large worst-case noise margin at a supply voltage below 0.6 V.

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  • 140.
    Tehrani, Payman
    et al.
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Kanciurzewska, Anna
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Crispin, Xavier
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Robinson, Nathaniel D.
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, The Institute of Technology.
    Fahlman, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, The Institute of Technology.
    Berggren, Magnus
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    The effect of pH on the elechtrochemical over-oxidation of PEDOT:PSS films2007In: Solid State Ionics, ISSN 0167-2738, E-ISSN 1872-7689, Vol. 177, no 39-40, p. 3521-3527Article in journal (Refereed)
    Abstract [en]

    Chemical degradation of conjugated polymers is one cause of material failures in polymer-based (opto)electronic devices, but can also be used as a technique for subtractive patterning of polymer films. When a large anodic potential is applied to the conducting polymer blend poly(3,4-ethylenedioxythiophene)-poly(4styrenesulfonate), PEDOT:PSS, an over-oxidation reaction occurs, altering its electrical conductivity. Here, we have studied the effect of pH on the electrochemical over-oxidation process of PEDOT in PEDOT:PSS. High pH is associated with a decrease of over-oxidation potential and an increase of resistivity in the resulting film. Vibrational spectroscopy and photoelectron spectroscopy measurements on over-oxidized PEDOT:PSS films indicate that the decrease in conductivity results from cleavage of the conjugation pathway accompanied by the formation of sulfone, carbonyl and carboxylic groups in the polymer chain.

  • 141.
    Tordera, Daniel
    et al.
    Linköping University, Department of Science and Technology. Linköping University, Faculty of Science & Engineering.
    Zhao, Dan
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Volkov, Anton
    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.
    Jonsson, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Thermoplasmonic Semitransparent Nanohole Electrodes2017In: Nano letters (Print), ISSN 1530-6984, E-ISSN 1530-6992, Vol. 17, no 5, p. 3145-3151Article in journal (Refereed)
    Abstract [en]

    Nonradiative decay of plasmons in metallic nanostructures offers unique means for light-to-heat conversion at the nanoscale. Typical thermoplasmonic systems utilize discrete particles, while metal nanohole arrays were instead considered suitable as heat sinks to reduce heating effects. By contrast, we show for the first time that under uniform broadband illumination (e.g., the sun) ultrathin plasmonic nanohole arrays can be highly competitive plasmonic heaters and provide significantly higher temperatures than analogous nanodisk arrays. Our plasmonic nanohole arrays also heat significantly more than nonstructured metal films, while simultaneously providing superior light transmission. Besides being efficient light-driven heat sources, these thin perforated gold films can simultaneously be used as electrodes. We used this feature to develop "plasmonic thermistors" for electrical monitoring of plasmon-induced temperature changes. The nanohole arrays provided temperature changes up to 7.5 K by simulated sunlight, which is very high compared to previously reported plasmonic systems under similar conditions (solar illumination and ambient conditions). Both temperatures and heating profiles quantitatively agree with combined optical and thermal simulations. Finally, we demonstrate the use of a thermoplasmonic nanohole electrode to power the first hybrid plasmonic ionic thermoelectric device, resulting in strong solar-induced heat gradients and corresponding thermoelectric voltages.

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  • 142.
    Toss, Henrik
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Suspene, Clement
    University of Paris Diderot, France .
    Piro, Benoit
    University of Paris Diderot, France .
    Yassar, Abderrahim
    Ecole Polytechnique, Palaiseau, France.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Kergoat, Loig
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Pham, Minh-Chau
    University of Paris Diderot, France .
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    On the mode of operation in electrolyte-gated thin film transistors based on different substituted polythiophenes2014In: Organic electronics, ISSN 1566-1199, E-ISSN 1878-5530, Vol. 15, no 10, p. 2420-2427Article in journal (Refereed)
    Abstract [en]

    Organic Thin Film Transistors (OTFT), gated through an aqueous electrolyte, have extensively been studied as sensors in various applications. These water-gated devices are known to work both as electrochemical (Organic ElectroChemical Transistor - OECT) and field-effect (Organic Field-Effect Transistor - OFET) devices. To properly model and predict the response of water-gated OTFT sensors it is important to distinguish between the mechanism, field-effect or electrochemical, by which the transistor is modulated and thus how the gate signal can be affected by the analyte. In this present study we explore three organic polymer semiconductors, poly-(3-hexyl-thiophene) (P3HT), poly-(3-carboxypentyl-thiphene) (P3CPT) and a co-polymer P3HT-co-poly-(3-ethoxypentanoic acid-thiophene) (monomer ratio 1:6, P3HT-COOH15) in water-gated OTFT structures. We report a set of transistor characteristics, including standard output parameters, impedance spectroscopy and current transients, to investigate the origin of the mode of operation in these water-gated OTFTs. Impedance characteristics, including both frequency and voltage dependence, were recorded for capacitor stacks corresponding to the gate/electrolyte/semiconductor/source structure. It is shown that P3HT as well as P3HT-COOH15 both can function as semiconductors in water gated OTFT devices operating in field-effect mode. P3CPT on the other hand shows typical signs of electrochemical mode of operation. The -COOH side group has been suggested as a possible anchoring site for biorecognition elements in EGOFET sensors, rendering P3HT-COOH15 a possible candidate for such applications.

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  • 143.
    Tran Nguyen, Ha
    et al.
    University Mons UMONS.
    Coulembier, Olivier
    University Mons UMONS.
    De Winter, Julien
    University Mons UMONS.
    Gerbaux, Pascal
    University Mons UMONS.
    Crispin, Xavier
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Dubois, Philippe
    University Mons UMONS.
    Novel regioregular poly(3-hexylthiophene)-based polycationic block copolymers2011In: POLYMER BULLETIN, ISSN 0170-0839, Vol. 66, no 1, p. 51-64Article in journal (Refereed)
    Abstract [en]

    Regioregular poly(3-hexylthiophene) has been successfully incorporated into various poly(N,N-dimethylamino-2-ethyl methacrylate)-based block copolymers, i.e., P3HT-b-PDMAEMA, via Grignard metathesis (GRIM) method and atom transfer radical polymerization (ATRP) reactions. The structure of the diblock copolymers was fully confirmed by FT-IR, H-1 NMR spectroscopy, gel permeation chromatography (GPC), and ultraviolet-visible spectroscopy (UV-vis). The recovered copolymers could be treated by protonation of the pending tertiary amine functions and depending on the relative content in PDMAEMA, the copolymers could be solubilized in more polar solvents where P3HT alone proved to be totally insoluble.

  • 144.
    Tu, Deyu
    et al.
    Linköping University, Department of Electrical Engineering, Information Coding. Linköping University, The Institute of Technology.
    Forchheimer, Robert
    Linköping University, Department of Electrical Engineering, Information Coding. Linköping University, The Institute of Technology.
    Herlogsson, Lars
    Linköping University, The Institute of Technology. Linköping University, Department of Science and Technology, Physics and Electronics.
    Crispin, Xavier
    Linköping University, The Institute of Technology. Linköping University, Department of Science and Technology, Physics and Electronics.
    Berggren, Magnus
    Linköping University, The Institute of Technology. Linköping University, Department of Science and Technology, Physics and Electronics.
    Parameter extraction for electrolyte-gated organic field effect transistor modeling2011Conference paper (Refereed)
    Abstract [en]

    We present a methodology to extract parameters for an electrolyte-gated organic field effect transistor DC model. The model is based on charge drift/diffusion transport under electric field and covers all regimes. Voltage dependent capacitance, mobility, contact resistance and threshold voltage shift are taken into account in this model. The feature parameters in the model are simply extracted from the transfer or output characteristics of electrolyte-gated organic field effect transistors. The extracted parameters are verified by good agreements between experimental and simulated results.

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  • 145.
    Tu, Deyu
    et al.
    Linköping University, The Institute of Technology. Linköping University, Department of Electrical Engineering, Information Coding.
    Herlogsson, Lars
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Kergoat, Loig
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Crispin, Xavier
    Linköping University, The Institute of Technology. Linköping University, Department of Science and Technology, Physics and Electronics.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    A Static Model for Electrolyte-Gated Organic Field-Effect Transistors2011In: IEEE Transactions on Electron Devices, ISSN 0018-9383, E-ISSN 1557-9646, Vol. 58, no 10, p. 3574-3582Article in journal (Refereed)
    Abstract [en]

    We present a dc model to simulate the static performance of electrolyte-gated organic field-effect transistors. The channel current is expressed as charge drift transport under electric field. The charges accumulated in the channel are considered being contributed fromvoltage-dependent electric-doublelayer capacitance. The voltage-dependent contact effect and short-channel effect are also taken into account in this model. A straightforward and efficient methodology is presented to extract the model parameters. The versatility of this model is discussed as well. The model is verified by the good agreement between simulation and experimental data.

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  • 146.
    Tu, Deyu
    et al.
    Linköping University, Department of Electrical Engineering, Information Coding. Linköping University, Faculty of Science & Engineering.
    Kergoat, Loïg
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering. Norrköping Sweden.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering. Norrköping Sweden.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering. Norrköping Sweden.
    Forchheimer, Robert
    Linköping University, Department of Electrical Engineering, Information Coding. Linköping University, Faculty of Science & Engineering.
    Transient analysis of electrolyte-gated organic field effect transistors2012In: SPIE Proceedings Vol. 8478: Organic Field-Effect Transistors XI / [ed] Zhenan Bao; Iain McCulloch, 2012, Vol. 8478, p. 84780L-1-84780L-8Conference paper (Refereed)
    Abstract [en]

    A terminal charge and capacitance model is developed for transient behavior simulation of electrolyte-gated organic field effect transistors (EGOFETs). Based on the Ward-Dutton partition scheme, the charge and capacitance model is derived from our drain current model reported previously. The transient drain current is expressed as the sum of the initial drain current and the charging current, which is written as the product of the partial differential of the terminal charges with respect to the terminal voltages and the differential of the terminal voltages upon time. The validity for this model is verified by experimental measurements.

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  • 147.
    Tzamalis, Georgios
    et al.
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, The Institute of Technology.
    Crispin, Xavier
    Linköping University, The Institute of Technology. Linköping University, Department of Science and Technology, Physics and Electronics.
    Andersson, Mats
    Chalmers.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Electrochemical control of amplified spontaneous emission in conjugated polymers2012In: Organic electronics, ISSN 1566-1199, E-ISSN 1878-5530, Vol. 13, no 6, p. 954-958Article in journal (Refereed)
    Abstract [en]

    We present a method of electrochemically tuning the threshold intensity of the amplified spontaneous emission (ASE) of a semiconducting polymer thin film. This can be achieved in close contact with a conducting polymer electrode (PEDOT:PSS), if the latter is electrochemically tuned to an optically transparent redox state for the emitted wavelength of interest. This electrical switch between ASE and fluorescence hints that a new route to achieve electrically pumped laser is by combining an electrochemical device with a lasing conjugated polymer.

  • 148.
    Tzamalis, Georgios
    et al.
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Lemaur, Vincent
    University Mons Hainaut.
    Karlsson, Fredrik
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
    Holtz, Per-Olof
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
    Andersson, Mats
    Chalmers.
    Crispin, Xavier
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Cornil, Jerome
    University Mons Hainaut.
    Berggren, Magnus
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Fluorescence light emission at 1 eV from a conjugated polymer2010In: CHEMICAL PHYSICS LETTERS, ISSN 0009-2614, Vol. 489, no 1-3, p. 92-95Article in journal (Refereed)
    Abstract [en]

    While polymer light-emitting diodes are currently finding commercial applications in displays and lighting, the development of low bandgap polymers emitting in the infrared has received much less attention in spite of potential applications for instance in the field of communication technologies. We report here a light emission at 1 eV from a low bandgap polymer made of an alternation of dialkoxy-phenylene units and a low bandgap monomer composed of an electron accepting 2-thia-1,3,5,8-tetraaza-cyclopenta[b]naphthalene group fenced with electron donating thiophene units. The electronic structure of the polymer chains has been characterized at a quantum-chemical level to shed light into the experimental results.

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  • 149.
    Ullah Khan, Zia
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Bubnova, Olga
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering. Optoelectronics Group, Cavendish Laboratory, University of Cambridge, Cambridge, UK.
    Jafari, Mohammad Javad
    Linköping University, Department of Physics, Chemistry and Biology, Molecular Physics. Linköping University, Faculty of Science & Engineering.
    Brooke, Robert
    Linköping University, Faculty of Science & Engineering. Linköping University, Department of Science and Technology, Physics and Electronics. University of South Australia, Mawson Institute, Mawson Lakes 5095, Australia.
    Liu, Xianjie
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering.
    Gabrielsson, Roger
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Ederth, Thomas
    Linköping University, Department of Physics, Chemistry and Biology, Molecular Physics. Linköping University, Faculty of Science & Engineering.
    Evans, Drew R.
    University of South Australia, Mawson Institute, Australia.
    Andreasen, Jens W.
    Technical University of Denmark, Department of Energy Conversion and Storage, Roskilde, Denmark.
    Fahlman, Mats
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Acido-basic control of the thermoelectric properties of poly(3,4-ethylenedioxythiophene)tosylate (PEDOT-Tos) thin films2015In: Journal of Materials Chemistry C, ISSN 2050-7526, E-ISSN 2050-7534, Vol. 3, p. 10616-10623Article in journal (Refereed)
    Abstract [en]

    PEDOT-Tos is one of the conducting polymers that displays the most promising thermoelectric properties. Until now, it has been utterly difficult to control all the synthesis parameters and the morphology governing the thermoelectric properties. To improve our understanding of this material, we study the variation in the thermoelectric properties by a simple acido-basic treatment. The emphasis of this study is to elucidate the chemical changes induced by acid (HCl) or base (NaOH) treatment in PEDOT-Tos thin films using various spectroscopic and structural techniques. We could identify changes in the nanoscale morphology due to anion exchange between tosylate and Cl- or OH-. But, we identified that changing the pH leads to a tuning of the oxidation level of the polymer, which can explain the changes in thermoelectric properties. Hence, a simple acid-base treatment allows finding the optimum for the power factor in PEDOT-Tos thin films.

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  • 150.
    Ullah Khan, Zia
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Edberg, Jesper
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Max Hamedi, Mahiar
    KTH Royal Institute Technology, Sweden.
    Gabrielsson, Roger
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Granberg, Hjalmar
    Innventia AB, Sweden.
    Wågberg, Lars
    KTH Royal Institute Technology, Sweden.
    Engquist, Isak
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    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.
    Thermoelectric Polymers and their Elastic Aerogels2016In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 28, no 22, p. 4556-4562Article in journal (Refereed)
    Abstract [en]

    Electronically conducting polymers constitute an emerging class of materials for novel electronics, such as printed electronics and flexible electronics. Their properties have been further diversified to introduce elasticity, which has opened new possibility for "stretchable" electronics. Recent discoveries demonstrate that conducting polymers have thermoelectric properties with a low thermal conductivity, as well as tunable Seebeck coefficients - which is achieved by modulating their electrical conductivity via simple redox reactions. Using these thermoelectric properties, all-organic flexible thermoelectric devices, such as temperature sensors, heat flux sensors, and thermoelectric generators, are being developed. In this article we discuss the combination of the two emerging fields: stretchable electronics and polymer thermoelectrics. The combination of elastic and thermoelectric properties seems to be unique for conducting polymers, and difficult to achieve with inorganic thermoelectric materials. We introduce the basic concepts, and state of the art knowledge, about the thermoelectric properties of conducting polymers, and illustrate the use of elastic thermoelectric conducting polymer aerogels that could be employed as temperature and pressure sensors in an electronic-skin.

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