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  • 151.
    Crispin, Xavier
    et al.
    University of Mons, Belgium.
    Bureau, C.
    CEA Saclay, France;.
    Geskin, V. M.
    University of Mons, Belgium.
    Lazzaroni, R.
    University of Mons, Belgium.
    Salaneck, William R.
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, The Institute of Technology.
    Bredas, J. L.
    University of Mons, Belgium.
    Chemisorption of acrylonitrile on the Cu(100) surface: A local density functional study1999In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 111, no 7, p. 3237-3251Article in journal (Refereed)
    Abstract [en]

    The possibility of chemically grafting polyacrylonitrile onto transition metal electrodes via electropolymerization leads to promising applications in the fields of corrosion protection or metal surface functionalization. The initial step of the electrografting mechanism is the adsorption of the acrylonitrile monomer on the metal surface from solution. Here, we investigate theoretically this adsorption process on the copper (100) surface; Density Functional Theory is used in the Local Spin Density approximation to describe the electronic and structural properties of acrylonitrile adsorbed on copper clusters. The chemisorption of acrylonitrile on the copper surface is confirmed experimentally via X-Ray Photoelectron Spectroscopy. The thermodynamic characteristics of the adsorption process are also studied via statistical mechanics. Finally, determining the influence of the copper cluster size on the adsorption of acrylonitrile allows to extrapolate the properties of the acrylonitrile/Cu(100) surface from those of acrylonitrile/copper clusters. (C) 1999 American Institute of Physics. [S0021-9606(99)70231-X].

  • 152.
    Crispin, X
    et al.
    University of Mons, Belgium;.
    Lazzaroni, R
    University of Mons, Belgium; .
    Geskin, V
    University of Mons, Belgium; .
    Baute, N
    University of Liege, Belgium;.
    Dubois, P
    University of Liege, Belgium; .
    Jerome, R
    University of Liege, Belgium; .
    Bredas, JL
    University of Mons, Belgium; .
    Controlling the electrografting of polymers onto transition metal surfaces through solvent vs monomer adsorption1999In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 121, no 1, p. 176-187Article in journal (Refereed)
    Abstract [en]

    Electropolymerization of methacrylic monomers opens the possibility of chemically grafting a wide range of polymers onto transition metal surfaces. In this work, the electropolymerization of polyacrylonitrile and polyethyl acrylate is studied in different solvents; we experimentally confirm that the choice of solvent is a critical parameter for obtaining electrografted polymers. A density-functional theory-based study modeling the interaction of solvent (acetonitrile, dimethylformamide, and pyridine) or monomer (acrylonitrile and ethyl acrylate) molecules with the Ni(100) metal surface provides the means to classify the organic molecules with respect to their ability to interact with the surface. The surface binding-energy difference between monomer and solvent is introduced in a Frumkin-type isotherm. This allows us to rationalize the experimental observations in terms of a competitive adsorption at the metal surface between the monomer and the solvent. The first step in the electrografting mechanism thus appears to be the chemisorption of the monomer at the electrode surface before cathodic polarization is applied; the chemisorbed monomer is therefore the first species reduced, giving rise to an adsorbed reactive intermediate, which is thus able to start the polymerization of a grafted chain.

  • 153.
    Johansson, N.
    et al.
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, The Institute of Technology.
    Osada, T.
    Sumitomo Chem Co Ltd, Japan.
    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.
    Parente, V.
    Mons University, Belgium.
    dos Santos, D. A.
    Mons University, Belgium.
    Crispin, Xavier
    Mons University, Belgium.
    Bredas, J. L.
    Mons University, Belgium.
    Electronic structure of tris(8-hydroxyquinoline) aluminum thin films in the pristine and reduced states1999In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 111, no 5, p. 2157-2163Article in journal (Refereed)
    Abstract [en]

    The electronic structure of tris(8-hydroxyquinoline) aluminum (Alq(3)) has been studied in the pristine molecular solid state as well as upon interaction (doping) with potassium and lithium. We discuss the results of a joint theoretical and experimental investigation, based on a combination of x-ray and ultraviolet photoelectron spectroscopies with quantum-chemical calculations at the density functional theory level. Upon doping, each electron transferred from an alkali metal atom is stored on one of the three ligands of the Alq(3) molecule, resulting in a new spectral feature (peak) in the valence band that evolves uniformly when going from a doping level of one to three metal atoms per Alq(3) molecule. (C) 1999 American Institute of Physics. [S0021-9606(99)50628-4].

  • 154.
    Crispin, Xavier
    et al.
    University of Mons, Belgium.
    Bureau, Christophe
    CEA Saclay, France.
    Geskin, Victor
    University of Mons, Belgium.
    Lazzaroni, Roberto
    University of Mons, Belgium.
    Bredas, Jean-Luc
    University of Mons, Belgium .
    Local density functional study of copper clusters: A comparison between real clusters, model surface clusters, and the actual metal surface1999In: European Journal of Inorganic Chemistry, ISSN 1434-1948, E-ISSN 1099-1948, no 2, p. 349-360Article in journal (Refereed)
    Abstract [en]

    Density Functional Theory is used to study the influence of the size of copper clusters modeling the Cu(100) surface, on the electronic properties: ionization potential, electron affinity, electronic chemical potential, and chemical hardness. The model clusters are chosen to have a bilayer structure and range in size from 9 to 20 copper atoms. The chemical hardness being identified as the relaxation energy of the frontier levels when an electron is removed or added to the system, a simple expression is proposed to estimate its value from the eigenenergies of the frontier levels in neutral and partially ionized systems. A detailed comparison of the geometric and electronic structures is made between the model surface copper clusters, real copper clusters, and the actual metal surface; it is seen that the model surface clusters provide an easy extrapolation to the properties of the metal surface.

  • 155.
    Cornil, J
    et al.
    University of Mons, Belgium.
    dos Santos, DA
    University of Mons, Belgium.
    Crispin, X
    University of Mons, Belgium.
    Silbey, R
    MIT, USA.
    Bredas, JL
    University of Mons, Belgium.
    Influence of interchain interactions on the absorption and luminescence of conjugated oligomers and polymers: A quantum-chemical characterization1998In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 120, no 6, p. 1289-1299Article in journal (Refereed)
    Abstract [en]

    Correlated quantum-chemical calculations are used to investigate the influence of interchain interactions on the absorption and emission of pi-conjugated chains. The results are discussed in relation to the utilization of conjugated materials as active elements in electro-optic devices; they provide guidelines on how to prevent a substantial decrease in luminescence yield in solid films. In high-symmetry cofacial configurations, interchain interactions lead to a blue shift of the lowest optical transition compared to that calculated for an isolated chain; the appearance of an additional red-shifted component is expected when positional disorder is considered. The absence of any significant oscillator strength in the transition between the ground state and the lowest excited state in highly symmetric complexes implies that the luminescence emission will be strongly quenched. This picture is. however, modified when one takes account of the relaxation processes which occur in the lowest excited state. The nature of the most stable photogenerated species and the role played by chemical impurities are also addressed.

  • 156.
    Bubnova, Olga
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Ullah Khan, Zia
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Wang, Hui
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Dagnelund, Daniel
    Linköping University, Department of Physics, Chemistry and Biology, Functional Electronic Materials. Linköping University, The Institute of Technology.
    Arlin, Jean-Baptiste
    Free University of Brussels Laboratoire de Chimie des Polymères, Bruxelles, Belgium.
    Geerts, Yves
    Free University of Brussels Laboratoire de Chimie des Polymères, Bruxelles, Belgium.
    Desbief, Simon
    University of Mons Laboratoire de chimie des materiaux nouveaux, Mons, Belgium.
    Breiby, Dag W.
    Department of Physics, Norwegian University of Science and Technology (NTNU), Trondheim, Norway.
    Andreasen, Jens W.
    Imaging and Structural Analysis Programme, Department of Energy Conversion and Storage, Technical University of Denmark, Roskilde, Denmark.
    Lazzaroni, Roberto
    University of Mons Laboratoire de chimie des materiaux nouveaux, Mons, Belgium.
    Zozoulenko, Igor
    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.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Advantageous thermoelectric properties of a semimetallic polymerManuscript (preprint) (Other academic)
    Abstract [en]

    Thermoelectric generation potentially holds a solution for waste heat recovery issues provided that the availability of inexpensive, biodegradable and highly efficient thermoelectric materials is insured in the near future. Plastic thermoelectrics could successfully comply with the said requirements if the thermoelectric efficiency (ZT) of conducting polymers was higher. However, given the novelty of the subject, at present there are no clear guidelines for ZT optimization in this class of materials. The most important piece of information that is currently missing is the description of a specific electronic makeup that conducting polymers must possess in order to enable good thermoelectric performance. In the present study the thermoelectric properties of poly(3,4-ethylenedioxythiophene) derivatives with two types of counterions, i.e. poly(styrenesulfonate) (PSS) and tosylate (Tos) are evaluated. A striking variation in their thermoelectric performance is attributed to structural and morphological differences between two polymers that manifest itself in dissimilar charge transport mechanism. The superior properties of PEDOT-Tos presumably originate from a high degree of crystallinity and structural order that predetermines the tendency for bipolaron band formation. Unlike polaronic PEDOT-PSS with slowly varying density of localized states (DOS) near the Fermi level (EF), the DOS in PEDOT-Tos is characterized by higher asymmetry and higher charge carrier density at EF (similar to semimetals), which allows for higher thermopower and electrical conductivity. Therefore, we conclude that the polymers with semimetallic electronic makeup are expected to exhibit promising thermoelectric properties with bigger variation in thermopower upon doping.

  • 157.
    Jakobsson, Fredrik L. E.
    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.
    Berggren, Magnus
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Filamentary switching of Rose Bengal devicesManuscript (preprint) (Other academic)
    Abstract [en]

    Switch devices with a structure of metal / orgamc layer / metal were fabricated, with the organic layer being Rose Bengal sodium salt, Rose Bengal bis(tricthylammonium) salt, Rose Bengal lactone and Fluorescein. All devices showed reversible switch behavior, ruling out electro reduction or conformational switching. Furthermore, only devices with ITO as substrate and Al or Ag as top electrode showed reversible switch behavior. Electrical characterization of the ITO substrate indicated that the switching is due to the reversible formation of conducting filaments, initiated from the ITO.

  • 158.
    Wang, Xiaodong
    et al.
    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.
    Improving the stability of water-gated organic transistors for sensing applicationsManuscript (preprint) (Other academic)
    Abstract [en]

    The instability of water-gated organic transistors is a major obstacle for their sensing applications in aqueous media. In the present work, we demonstrate that adding a fluorinated ion exchange membrane, Nafion, on a water-gated organic transistor can increase significantly the stability of the device to air exposure. In addition, choosing a suitable operating voltage range, e.g. Vg=0 ↔ -0.7 V, is shown to be crucial for achieving stable (repeatable) measurements in aqueous media. It is also feasible to exploit this kind of transistor as a chemical sensor to discriminate different chemicals which are dissolved in water.

  • 159.
    Bubnova, Olga
    et al.
    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.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Ph effect on thermoelectric properties of poly-(3,4-ethylenedioxythiophene):tosylateManuscript (preprint) (Other academic)
    Abstract [en]

    Abstract not available.

  • 160.
    Wang, Xiaodong
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology.
    Platt, Duncan
    Acreo AB, Norrköping, Sweden.
    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.
    Printed low loss capacitors for use in a wireless humidity sensor labelManuscript (preprint) (Other academic)
    Abstract [en]

    A low loss printed capacitor is achieved by using a screen printable benzocyclobutene-based solution. The dissipation factor is measured to be 0.001 at frequencies around 3 MHz, which is low compared to commercially available dielectric inks with dissipation factors of ~0.05 in the same frequency region. By incorporating low loss printed capacitors with a planar antenna and a printed humidity sensor capacitor, a humidity sensor label which resonates at 3 MHz is demonstrated. The label is fully printed on a flexible substrate pre-patterned with the antenna and the manufacturing process is compatible with low-cost reelto-reel processing technology. The quality factor (Q factor) of the sensor label is enhanced up to about 15 in ambient environment. This allows readout of the sensor response at a distance and through damping materials such as walls in a building.

  • 161.
    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.))
  • 162.
    Wadeasa, Amal
    et al.
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Tzamalis, G.
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Nour, Omer
    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.
    Willander, Magnus
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Solution processed ZnO nanorods/polyfluorene semiconductor heterojunctions with white light photoluminescenceManuscript (preprint) (Other academic)
    Abstract [en]

    Hybrid inorganic-organic semiconductor heterojunctions are nowadays scrutinized for optoelectronic devices, such as solar cells and light emitting diodes. Here, ZnOnanorods/ polyfluorene heterojunctions have been entirely fabricated from solution by wet chemistry and low temperature processes. The morphology of the polyfluorene film appears to be an important parameter to control the growth of the ZnO nanorods and affects their optical properties. The visible emission of the conjugated polymer and the ZnO are complementary and provide a broad emission in the visible. Because of its solution processability and broad emission, the ZnO/polyfluorene heterojunction is promising for large area white lightning applications.

  • 163.
    Bao, Qinye
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Andersson, Mattias
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Braun, Slawomir
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Sun, Zhengyi
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. 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.
    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.
    The energetics of the semiconducting polymer-electrode interface for solution-processed electronicsManuscript (preprint) (Other academic)
    Abstract [en]

    The semiconductor-electrode interface impacts the function and the performance of (opto-)electronic devices. For printed organic electronics the electrode surface is not atomically clean leading to weakly interacting interfaces. As a result, solution-processed organic ultra-thin films on electrodes typically form islands due to de-wetting. It has therefore been utterly difficult to achieve homogenous ultrathin conjugated polymer films. This has made the investigation of the correct energetics of the conjugated polymer-electrode interface impossible. Also, this has hampered the development of devices including ultra-thin conjugated polymer layers. Here, we report Langmuir-Shäfer-manufactured homogenous mono- and multilayers of semiconducting polymers on metal electrodes and track the energy level bending using photoelectron spectroscopy. The amorphous films display an abrupt energy level bending that does not extend beyond the first monolayer. Our findings provide new insights of the energetics of the polymer-electrode interface and opens up for new high-performing devices based on ultra-thin semiconducting polymers.

  • 164.
    Jakobsson, Fredrik L. E.
    et al.
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Marsal, Philippe
    Laboratory for Chemistry of Novel Materials, University of Mons-Hainaut, Place du Parc 20, B-7000 Mons, Belgium.
    Braun, Slawomir
    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.
    Cornil, Jérôme
    Laboratory for Chemistry of Novel Materials, University of Mons-Hainaut, Place du Parc 20, B-7000 Mons, Belgium.
    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.
    Tuning the energy levels of photochromic diarylethene compounds for optoelectronic switch devicesManuscript (Other academic)
    Abstract [en]

    Photochromic diarylethene molecules (PC) is investigated for use in opticalwrite/electrical read memory applications. The frontier energy levels and dipolemoment is calculated using density functional theory. Good agreement is foundbetween calculated electronic structure and measured ultraviolet photoelectronspectra. The changes in frontier energy levels and dipole moment are scrutinizedupon two different approaches for chemical modification: (i) adding substituentsto the ethylene bridge; or (ii) changing the chemical nature of the aryl rings.Through the chemical modification the frontier energy levels can be tuned bymore than 2 eV. The calculated molecular properties are used in charge transportmodels to predict the behavior of devices based on these molecules. By using thePC in combination with an organic semiconductor (in bilayer or blend) goodswitching behavior can be achieved in a device. The switch effect is predicted tobe mainly due to switch in frontier energy levels rather than switch of dipolemoment. This is concluded since the dipole moment is either too small (< 5 D) orthe switch effect to small (less than a factor of two).

  • 165.
    Larsson, Oscar
    et al.
    Linköping University, Department of Science and Technology. Linköping University, The Institute of Technology.
    Laiho, Ari
    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.
    Unifying electrochemical and field-effect mechanisms in electrolyte-gated organic field-effect transistorsManuscript (preprint) (Other academic)
    Abstract [en]

    The combination of electrolytes and organic semiconductors has opened up new opportunities in photonics1, electronics2 and in energy storage3. In most of these devices, the key mechanisms involve the transport of charge carriers (electrons or ions) across the organic semiconductor-electrolyte interface. The formation of an electric double layer (EDL) at this polarized interface is fuzzier than at a metal-electrolyte interface since weak intermolecular interactions in the organic solid favour the penetration of ions4. An EDL established at the organic semiconductor-electrolyte interface, defined by a sheet of electronic charge carriers and a sheet of ions, has been proposed recently as the basic mechanism for electrolyte-gated organic field-effect transistors (EGOFETs)5, 6. Here, organic thin film transistors are used as a probe to investigate the organic semiconductor-electrolyte interface. We demonstrate that the capacitance value of the gate counter electrode dictates the degree of advancement7 of the electrochemical halfreaction (the extent of the reaction) at this interface. This finding unifies the mechanisms proposed for EGOFETs and organic electrochemical transistors (OECTs); and sets the ground description for an electrochemical half-reaction induced entirely by capacitive coupling.

  • 166.
    Hansson (f.d. Wadeasa), Amal
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology. null.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology. null.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology. null.
    ZnO-Polymer hybrid electron only rectifiersManuscript (preprint) (Other academic)
    Abstract [en]

    The combination of organic semiconductors and ZnO nanorods provides new hybrid devices for large area optoelectronics targeting solar energy harvesting and light emission applications. The electronic transport across organic-ZnO heterojunction is not well understood. Here, we investigate systematically the creation of the ZnOpolymer interface and pinpoint potential issues in hybrid devices based on chemically grown ZnO nanorods. For the sake of simplicity, we focus on a ZnO-polymer hybrid device transporting only electrons. The semiconducting polymer used is poly {[N,N0-bis(2-octyldodecyl)-naphthalene-1,4,5,8-bis(dicarboximide)-2,6-diyl]-alt-5,50-(2,20-dithiophene)}. The device shows easy electron injection from Au/ZnO contacts and a good rectification partially governed by the morphology of the heterojunction.

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