Modelling charge transport in organic semiconductors: from quantum dynamics to soft matter.

The charge carrier dynamics in organic semiconductors has been traditionally discussed with the models used in inorganic crystalline and amorphous solids but this analogy has severe limitations because of the more complicated role of nuclear motions in organic materials. In this perspective, we discuss how a new approach to the modelling of charge transport is emerging from the alliance between the conventional quantum chemical methods and the methods more traditionally used in soft-matter modelling. After describing the conventional limit cases of charge transport we discuss the problems arising from the comparison of the theory with the experimental and computational results. Several recent applications of numerical methods based on the propagation of the wavefunction or kinetic Monte Carlo methods on soft semiconducting materials are reviewed.

[1]  M. Koeberg,et al.  On the mechanism of charge transport in pentacene. , 2008, The Journal of chemical physics.

[2]  J. Nelson,et al.  Simulating charge transport in tris(8-hydroxyquinoline) aluminium (Alq(3)). , 2008, Physical chemistry chemical physics : PCCP.

[3]  R. Silbey,et al.  A unified theory for charge-carrier transport in organic crystals. , 2008, The Journal of chemical physics.

[4]  K. Pernstich,et al.  Field-effect-modulated Seebeck coefficient in organic semiconductors. , 2008, Nature materials.

[5]  C. Zannoni,et al.  "Reduced" distributed monopole model for the efficient prediction of energy transfer in condensed phases. , 2008, The journal of physical chemistry. B.

[6]  Ferdinand C. Grozema,et al.  Mechanism of charge transport in self-organizing organic materials , 2008 .

[7]  C. Rothe.  Electrical doping is paving the way for the implementation of OLEDs in consumer electronics , 2007 .

[8]  Wojciech Pisula,et al.  Discotic liquid crystals: a new generation of organic semiconductors. , 2007, Chemical Society reviews.

[9]  F. Lelj,et al.  Atomistic simulation of discotic liquid crystals: transition from isotropic to columnar phase example. , 2007, The Journal of chemical physics.

[10]  A. Troisi,et al.  Prediction of the Absolute Charge Mobility of Molecular Semiconductors: the Case of Rubrene , 2007 .

[11]  David Curcó,et al.  Computational tool to model the packing of polycyclic chains: Structural analysis of amorphous polythiophene , 2007, J. Comput. Chem..

[12]  Z. Shuai,et al.  Roles of inter- and intramolecular vibrations and band-hopping crossover in the charge transport in naphthalene crystal. , 2007, The Journal of chemical physics.

[13]  B. Batlogg,et al.  Large uniaxial negative thermal expansion in pentacene due to steric hindrance , 2007, 0707.0450.

[14]  F. Bechstedt,et al.  Ab initio studies of structural, vibrational, and electronic properties of durene crystals and molecules , 2007 .

[15]  J. Nelson,et al.  Predictive study of charge transport in disordered semiconducting polymers. , 2007, Nano letters.

[16]  J. Gierschner,et al.  Liquid crystalline octaalkoxycarbonyl phthalocyanines: design, synthesis, electronic structure, self-aggregation and mesomorphism , 2007 .

[17]  C. Zannoni,et al.  Molecular properties and stacking of 1-substituted hexaalkoxy triphenylenes , 2007 .

[18]  M. Bendikov,et al.  Twisting of conjugated oligomers and polymers: case study of oligo- and polythiophene. , 2007, Chemistry.

[19]  Henning Sirringhaus,et al.  Electron and ambipolar transport in organic field-effect transistors. , 2007, Chemical reviews.

[20]  Jean-Luc Brédas,et al.  Charge transport in organic semiconductors. , 2007, Chemical reviews.

[21]  Priya J. Jadhav,et al.  Electric-field-dependent percolation model of charge-carrier mobility in amorphous organic semiconductors , 2007 .

[22]  Sven Stafström,et al.  Impact of ring torsion on the intrachain mobility in conjugated polymers , 2007 .

[23]  A. Salleo.  Charge transport in polymeric transistors , 2007 .

[24]  Irwin Oppenheim,et al.  Chemical Dynamics in Condensed Phases , 2007 .

[25]  Kurt Kremer,et al.  Charge mobility of discotic mesophases: a multiscale quantum and classical study. , 2007, Physical review letters.

[26]  L. Zuppiroli,et al.  Quantum coherence and carriers mobility in organic semiconductors , 2006, cond-mat/0609454.

[27]  Ling Li,et al.  Temperature and field-dependence of hopping conduction in organic semiconductors , 2007, Microelectron. J..

[28]  T. Takenobu,et al.  Spatial extent of wave functions of gate-induced hole carriers in pentacene field-effect devices as investigated by electron spin resonance. , 2006, Physical review letters.

[29]  A. Morpurgo,et al.  Tunable Fröhlich polarons in organic single-crystal transistors , 2006, Nature materials.

[30]  John E Anthony,et al.  Functionalized acenes and heteroacenes for organic electronics. , 2006, Chemical reviews.

[31]  M. Ratner,et al.  Quantum chemical analysis of electronic structure and n- and p-type charge transport in perfluoroarene-modified oligothiophene semiconductors. , 2006, The journal of physical chemistry. B.

[32]  O. Ostroverkhova,et al.  Anisotropy of transient photoconductivity in functionalized pentacene single crystals , 2006 .

[33]  A. Cammidge.  The effect of size and shape variation in discotic liquid crystals based on triphenylene cores , 2006, Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences.

[34]  R. Weiss,et al.  Cis → trans and trans → cis isomerizations of styrylcoumarins in the solid state. Importance of the location of free volume in crystal lattices , 2006, Photochemical & photobiological sciences : Official journal of the European Photochemistry Association and the European Society for Photobiology.

[35]  L. Siebbeles,et al.  Charge transport along phenylenevinylene molecular wires , 2006 .

[36]  K. Kremer,et al.  Atomistic simulation of structure and dynamics of columnar phases of hexabenzocoronene derivatives. , 2006, The Journal of chemical physics.

[37]  Efficient charge transport along phenylene-vinylene molecular wires. , 2006, The journal of physical chemistry. B.

[38]  Edward F. Valeev,et al.  Effect of electronic polarization on charge-transport parameters in molecular organic semiconductors. , 2006, Journal of the American Chemical Society.

[39]  H. Bock,et al.  An Efficient Route to Stable Room-Temperature Liquid-Crystalline Triphenylenes , 2006 .

[40]  D. Bradley,et al.  Temperature and field dependence of hole mobility in poly(9,9-dioctylfluorene) , 2006 .

[41]  D. Schulz,et al.  Defect contributions to conductivity in poly(3‐hexylthiophene)? , 2006 .

[42]  N. Koch,et al.  Evidence for temperature-dependent electron band dispersion in pentacene. , 2006, Physical review letters.

[43]  Michael E. Gershenson,et al.  Ultrafast carrier dynamics in pentacene, functionalized pentacene, tetracene, and rubrene single crystals , 2006 .

[44]  Alessandro Troisi,et al.  Charge-transport regime of crystalline organic semiconductors: diffusion limited by thermal off-diagonal electronic disorder. , 2006, Physical review letters.

[45]  G. Wegner,et al.  Modeling of molecular packing and conformation in oligofluorenes. , 2006, The journal of physical chemistry. B.

[46]  M. Toney,et al.  Highly oriented crystals at the buried interface in polythiophene thin-film transistors , 2006 .

[47]  Junbiao Peng,et al.  First-principle band structure calculations of tris(8-hydroxyquinolinato)aluminum. , 2006, The journal of physical chemistry. B.

[48]  R. J. Kline,et al.  Morphology and Charge Transport in Conjugated Polymers , 2006 .

[49]  Alessandro Troisi,et al.  Dynamics of the intermolecular transfer integral in crystalline organic semiconductors. , 2005, The journal of physical chemistry. A.

[50]  C. Zannoni,et al.  Columnar and interdigitated structures from apolar discotic mesogens with radial dipoles: a Monte Carlo study , 2005 .

[51]  John E. Anthony,et al.  Electronic interactions and thermal disorder in molecular crystals containing cofacial pentacene units , 2005 .

[52]  Mark R. Wilson,et al.  Progress in computer simulations of liquid crystals , 2005 .

[53]  P. Blom,et al.  Unified description of charge-carrier mobilities in disordered semiconducting polymers. , 2005, Physical review letters.

[54]  R. Street,et al.  Transport in polycrystalline polymer thin-film transistors , 2005 .

[55]  Jean M. J. Fréchet,et al.  Dependence of Regioregular Poly(3-hexylthiophene) Film Morphology and Field-Effect Mobility on Molecular Weight , 2005 .

[56]  M. Ratner,et al.  Electronic structure and band gaps in cationic heterocyclic oligomers. Multidimensional analysis of the interplay of heteroatoms, substituents, molecular length, and charge on redox and transparency characteristics. , 2005, The journal of physical chemistry. B.

[57]  P. Dowben,et al.  The electronic structure of oriented poly[2-methoxy-5-(2’-ethyl-hexyloxy)- 1,4-phenylene-vinylene] , 2005 .

[58]  A. Troisi,et al.  Band structure of the four pentacene polymorphs and effect on the hole mobility at low temperature. , 2005, The journal of physical chemistry. B.

[59]  John E. Anthony,et al.  Bandlike transport in pentacene and functionalized pentacene thin films revealed by subpicosecond transient photoconductivity measurements , 2005 .

[60]  I. Chao,et al.  Effect of perfluorination on the charge-transport properties of organic semiconductors: density functional theory study of perfluorinated pentacene and sexithiophene , 2005 .

[61]  S. Clark,et al.  First-principles studies of the structural and electronic properties of poly-para-phenylene vinylene , 2004 .

[62]  Abhishek P. Kulkarni,et al.  Electron Transport Materials for Organic Light-Emitting Diodes , 2004 .

[63]  David Beljonne,et al.  Charge-transfer and energy-transfer processes in pi-conjugated oligomers and polymers: a molecular picture. , 2004, Chemical reviews.

[64]  W. R. Salaneck,et al.  Electronic delocalization in discotic liquid crystals: a joint experimental and theoretical study. , 2004, Journal of the American Chemical Society.

[65]  Michael A. Haase,et al.  Recent Progress in Organic Electronics: Materials, Devices, and Processes , 2004 .

[66]  Intrinsic hole mobility and trapping in a regioregular poly(thiophene) , 2004, cond-mat/0407502.

[67]  W. Fix,et al.  From polymer transistors toward printed electronics , 2004 .

[68]  Niyazi Serdar Sariciftci,et al.  Organic solar cells: An overview , 2004 .

[69]  C. Rovira,et al.  Correlation between crystal structure and mobility in organic field-effect transistors based on single crystals of tetrathiafulvalene derivatives. , 2004, Journal of the American Chemical Society.

[70]  G. Cinacchi,et al.  Atomistic molecular dynamics simulation of hexakis(pentyloxy)triphenylene: Structure and translational dynamics of its columnar state , 2004 .

[71]  Oana D. Jurchescu,et al.  Effect of impurities on the mobility of single crystal pentacene , 2004, cond-mat/0404130.

[72]  J. Brédas,et al.  A multimode analysis of the gas-phase photoelectron spectra in oligoacenes. , 2004, The Journal of chemical physics.

[73]  J. Rogers,et al.  Intrinsic charge transport on the surface of organic semiconductors. , 2004, Physical review letters.

[74]  Michael G Debije,et al.  The optical and charge transport properties of discotic materials with large aromatic hydrocarbon cores. , 2004, Journal of the American Chemical Society.

[75]  Qiang Huang,et al.  Computer simulation of long side-chain substituted poly(phenylene vinylene) polymers. , 2004, Chemphyschem : a European journal of chemical physics and physical chemistry.

[76]  Georg Kresse,et al.  Theory of polaron bandwidth narrowing in organic molecular crystals , 2004 .

[77]  K. Ogawa,et al.  X-ray diffraction analysis of nonequilibrium states in crystals: observation of an unstable conformer in flash-cooled crystals. , 2004, Journal of the American Chemical Society.

[78]  J. Brédas,et al.  Charge transport properties in discotic liquid crystals: a quantum-chemical insight into structure-property relationships. , 2004, Journal of the American Chemical Society.

[79]  D V Lang,et al.  Amorphouslike density of gap states in single-crystal pentacene. , 2004, Physical review letters.

[80]  E. Venuti,et al.  Organic Semiconductors: Polymorphism, Phonon Dynamics and Carrier-Phonon Coupling in Pentacene , 2003, cond-mat/0307115.

[81]  S. Ciuchi,et al.  Dynamical mean-field theory of transport of small polarons. , 2003, Physical review letters.

[82]  P. Blom,et al.  Unification of the hole transport in polymeric field-effect transistors and light-emitting diodes. , 2003, Physical review letters.

[83]  M. Winokur,et al.  Nanoscale structure–property relationships in conjugated polymers: Implications for present and future device applications , 2003 .

[84]  D. Bradley,et al.  Investigation of transport properties in polymer/fullerene blends using time-of-flight photocurrent measurements , 2003 .

[85]  K. Senthilkumar,et al.  Charge transport in columnar stacked triphenylenes: Effects of conformational fluctuations on charge transfer integrals and site energies , 2003 .

[86]  Jean M. J. Fréchet,et al.  Controlling the Field‐Effect Mobility of Regioregular Polythiophene by Changing the Molecular Weight , 2003 .

[87]  Stephen R. Forrest,et al.  Efficient bulk heterojunction photovoltaic cells using small-molecular-weight organic thin films , 2003, Nature.

[88]  S. Kelly,et al.  Liquid Crystals for Charge Transport, Luminescence, and Photonics , 2003 .

[89]  S. Sysoev,et al.  Single-crystal organic field effect transistors with the hole mobility ∼8 cm2/V s , 2003, cond-mat/0306192.

[90]  Guangming Wang,et al.  Increased mobility from regioregular poly(3-hexylthiophene) field-effect transistors , 2003 .

[91]  J. Ryckaert,et al.  Influence of shape and energy anisotropies on the phase diagram of discotic molecules. , 2003, Physical review. E, Statistical, nonlinear, and soft matter physics.

[92]  G. Kearley,et al.  Dynamics of a triphenylene discotic molecule, HAT6, in the columnar and isotropic liquid phases. , 2003, Journal of the American Chemical Society.

[93]  Yuan-Chung Cheng,et al.  Three-dimensional band structure and bandlike mobility in oligoacene single crystals: A theoretical investigation , 2003 .

[94]  G. Wijs,et al.  Anisotropy of the mobility of pentacene from frustration , 2003, cond-mat/0301078.

[95]  J. Brédas,et al.  Hole- and electron-vibrational couplings in oligoacene crystals: intramolecular contributions. , 2002, Physical review letters.

[96]  Lin H. Yang,et al.  Structural and electronic properties of pentacene molecule and molecular pentacene solid , 2002, cond-mat/0211420.

[97]  Florian Müller-Plathe,et al.  Coarse-graining in polymer simulation: from the atomistic to the mesoscopic scale and back. , 2002, Chemphyschem : a European journal of chemical physics and physical chemistry.

[98]  M. Itkis,et al.  Band electronic structure of one- and two-dimensional pentacene molecular crystals , 2002 .

[99]  M. Ratner,et al.  Intramolecular charge transport along isolated chains of conjugated polymers: Effect of torsional disorder and polymerization defects , 2002 .

[100]  Jean-Luc Brédas,et al.  Charge Transport in Discotic Liquid Crystals: A Molecular Scale Description , 2002 .

[101]  J. P. Calbert,et al.  Organic semiconductors: A theoretical characterization of the basic parameters governing charge transport , 2002, Proceedings of the National Academy of Sciences of the United States of America.

[102]  K. Ogawa,et al.  Invisible but common motion in organic crystals: a pedal motion in stilbenes and azobenzenes. , 2001, Journal of the American Chemical Society.

[103]  A. Troisi,et al.  The hole transfer in DNA: calculation of electron coupling between close bases , 2001 .

[104]  M. Chipara,et al.  Comparison of the π-conjugated ring orientations in polyaniline and polypyrrole , 2001 .

[105]  D. Morton-Blake,et al.  The thermochromism of poly(3-alkylthiophene)s: the role of the side chains , 2001 .

[106]  Crystal design of organic pigments — a prototype discipline of materials science , 2001 .

[107]  D. Morton-Blake,et al.  An atomistic simulation of the effect of pressure on conductive polymers , 2001 .

[108]  Y. Tokura,et al.  Hysteretic Thermochromism of Regioregular Poly(3-alkylthiophene) Thin Films , 2001 .

[109]  Richard L. Martin,et al.  Molecular geometry fluctuations and field-dependent mobility in conjugated polymers , 2001 .

[110]  D. Morton-Blake,et al.  Thermochromic distortions in a poly(3-alkylthiophene): an atomistic simulation investigation , 2000 .

[111]  O. Inganäs,et al.  Structural anisotropy of poly(alkylthiophene) films , 2000 .

[112]  Jiang,et al.  Two-dimensional electronic excitations in self-assembled conjugated polymer nanocrystals , 2000, Science.

[113]  A R Bishop,et al.  Molecular geometry fluctuation model for the mobility of conjugated polymers. , 2000, Physical review letters.

[114]  R. Silbey,et al.  Almost temperature independent charge carrier mobilities in liquid crystals , 2000 .

[115]  C. Zannoni,et al.  Columnar phases and field induced biaxiality of a Gay–Berne discotic liquid crystal , 2000 .

[116]  John M. Warman,et al.  Record Charge Carrier Mobility in a Room‐Temperature Discotic Liquid‐Crystalline Derivative of Hexabenzocoronene , 1999 .

[117]  E. W. Meijer,et al.  Two-dimensional charge transport in self-organized, high-mobility conjugated polymers , 1999, Nature.

[118]  George G. Malliaras,et al.  Temperature- and field-dependent electron and hole mobilities in polymer light-emitting diodes , 1999 .

[119]  Thomas N. Jackson,et al.  Pentacene organic thin-film transistors for circuit and display applications , 1999 .

[120]  Paul Ernest Parris,et al.  Essential Role of Correlations in Governing Charge Transport in Disordered Organic Materials , 1998 .

[121]  John M. Warman,et al.  MECHANISM OF CHARGE TRANSPORT ALONG COLUMNAR STACKS OF A TRIPHENYLENE DIMER , 1998 .

[122]  M. Lannoo,et al.  Electron-phonon coupling for aromatic molecular crystals: Possible consequences for their superconductivity , 1998 .

[123]  Mats Andersson,et al.  Laminated fabrication of polymeric photovoltaic diodes , 1998, Nature.

[124]  S. Forrest,et al.  Highly efficient phosphorescent emission from organic electroluminescent devices , 1998, Nature.

[125]  Mark R. Wilson,et al.  Molecular dynamics simulations of liquid crystal phases using atomistic potentials , 1998 .

[126]  C. Zannoni,et al.  Directional energy transfer in columnar liquid crystals: A computer-simulation study , 1998 .

[127]  John M. Warman,et al.  Highly mobile electrons and holes on isolated chains of the semiconducting polymer poly(phenylene vinylene) , 1998, Nature.

[128]  John W. Goodby,et al.  Handbook of liquid crystals , 1998 .

[129]  M. Vissenberg,et al.  Theory of the field-effect mobility in amorphous organic transistors , 1998, cond-mat/9802133.

[130]  Richard D. McCullough,et al.  THE CHEMISTRY OF CONDUCTING POLYTHIOPHENES , 1998 .

[131]  D. Morton-Blake,et al.  ATOMISTIC INVESTIGATION OF THERMOCHROMISM IN A POLY(3-ALKYLTHIOPHENE) , 1997 .

[132]  I. Brovchenko.  Lattice relaxation in molecular crystals with localized charges , 1997 .

[133]  Thomas N. Jackson,et al.  Pentacene-based organic thin-film transistors , 1997 .

[134]  C. Zannoni,et al.  MONTE CARLO SIMULATION OF DISCOTIC GAY-BERNE MESOGENS WITH AXIAL DIPOLE , 1997 .

[135]  Zhenan Bao,et al.  Soluble and processable regioregular poly(3‐hexylthiophene) for thin film field‐effect transistor applications with high mobility , 1996 .

[136]  K. Müllen,et al.  Columnar mesophases of alkylated hexa-peri-hexabenzocoronenes with remarkably large phase widths , 1996 .

[137]  Movaghar,et al.  Mechanism of charge transport in discotic liquid crystals. , 1995, Physical review. B, Condensed matter.

[138]  E. O. Arikainen,et al.  Effects of side-chain length on the charge transport properties of discotic liquid crystals and their implications for the transport mechanism , 1995 .

[139]  Roald Hoffmann,et al.  A THEORETICAL STUDY OF CRYSTALLOCHROMY. QUANTUM INTERFERENCE EFFECTS IN THE SPECTRA OF PERYLENE PIGMENTS , 1994 .

[140]  Conwell,et al.  First-principles calculation of the three-dimensional band structure of poly(phenylene vinylene). , 1993, Physical review. B, Condensed matter.

[141]  H. Bässler.  Charge Transport in Disordered Organic Photoconductors a Monte Carlo Simulation Study , 1993 .

[142]  T. Arias,et al.  Iterative minimization techniques for ab initio total energy calculations: molecular dynamics and co , 1992 .

[143]  S. Kondo,et al.  A Computational Approach to the Structure and Motion of Hexakis(pentyloxy)triphenylene(THE5) in Discotic Mesophase. , 1992 .

[144]  A. Maliniak.  Molecular dynamics of discotics in the isotropic phase , 1992 .

[145]  K. Yoshino,et al.  Structure and thermochromic solid‐state phase transition of poly (3‐alkylthiophene) , 1991 .

[146]  R. N. Marks,et al.  Light-emitting diodes based on conjugated polymers , 1990, Nature.

[147]  Campbell,et al.  First-principles calculations of the three-dimensional structure and intrinsic defects in trans-polyacetylene. , 1990, Physical review. B, Condensed matter.

[148]  Gilles Horowitz,et al.  A field-effect transistor based on conjugated alpha-sexithienyl , 1989 .

[149]  Campbell,et al.  Three-dimensional structure and intrinsic defects in trans-polyacetylene. , 1989, Physical review letters.

[150]  Dunlap,et al.  Unified theory of the mobilities of photoinjected electrons in naphthalene. , 1989, Physical review letters.

[151]  R. Nolte,et al.  Homologous series of liquid-crystalline metal free and copper octa-n-alkoxyphthalocyanines , 1989 .

[152]  W. R. Salaneck,et al.  Thermochromism in poly(3‐hexylthiophene) in the solid state: A spectroscopic study of temperature‐dependent conformational defects , 1988 .

[153]  R. Friend,et al.  New semiconductor device physics in polymer diodes and transistors , 1988, Nature.

[154]  Nevill Mott,et al.  Conduction in non-crystalline materials , 1989 .

[155]  R. Silbey,et al.  Theory of electronic transport in molecular crystals. II. Zeroth order states incorporating nonlocal linear electron–phonon coupling , 1985 .

[156]  W. Warta,et al.  Hot holes in naphthalene: High, electric-field-dependent mobilities. , 1985, Physical review. B, Condensed matter.

[157]  C. Jacoboni,et al.  The Monte Carlo method for the solution of charge transport in semiconductors with applications to covalent materials , 1983 .

[158]  B. Berne.  Modification of the overlap potential to mimic a linear site-site potential , 1981 .

[159]  Joshua Jortner,et al.  Temperature dependent activation energy for electron transfer between biological molecules , 1976 .

[160]  I. Vilfan.  Small polaron model of the electron motion in organic molecular crystals , 1973 .

[161]  T. Holstein,et al.  Studies of polaron motion: Part II. The “small” polaron , 1959 .

[162]  Rudolph A. Marcus,et al.  Electrostatic Free Energy and Other Properties of States Having Nonequilibrium Polarization. I , 1956 .

[163]  D. D. Eley.  Phthalocyanines as Semiconductors , 1948, Nature.