Achieving ideal transistor characteristics in conjugated polymer semiconductors

Organic thin-film transistors (OTFTs) with ideal behavior are highly desired, because nonideal devices may overestimate the intrinsic property and yield inferior performance in applications. In reality, most polymer OTFTs reported in the literature do not exhibit ideal characteristics. Supported by a structure-property relationship study of several low-disorder conjugated polymers, here, we present an empirical selection rule for polymer candidates for textbook-like OTFTs with high reliability factors (100% for ideal transistors). The successful candidates should have low energetic disorder along their backbones and form thin films with spatially uniform energetic landscapes. We demonstrate that these requirements are satisfied in the semicrystalline polymer PffBT4T-2DT, which exhibits a reliability factor (~100%) that is exceptionally high for polymer devices, rendering it an ideal candidate for OTFT applications. Our findings broaden the selection of polymer semiconductors with textbook-like OTFT characteristics and would shed light upon the molecular design criteria for next-generation polymer semiconductors.

[1]  D. He,et al.  Donor Engineering Tuning the Analog Switching Range and Operational Stability of Organic Synaptic Transistors for Neuromorphic Systems , 2022, Advanced Functional Materials.

[2]  Zhiqun Lin,et al.  Transforming Polymorphs via Meniscus-Assisted Solution-Shearing Conjugated Polymers for Organic Field-Effect Transistors. , 2022, ACS nano.

[3]  Yunlong Guo,et al.  A thriving decade: rational design, green synthesis, and cutting-edge applications of isoindigo-based conjugated polymers in organic field-effect transistors , 2022, Science China Chemistry.

[4]  Zhengke Li,et al.  Efficient n-Type Small-Molecule Mixed Ion-Electron Conductors and Application in Hydrogen Peroxide Sensors. , 2022, ACS applied materials & interfaces.

[5]  J. Pei,et al.  Building crystal structures of conjugated polymers through X‐ray diffraction and molecular modeling , 2021, SmartMat.

[6]  A. Pain,et al.  Rapid single-molecule detection of COVID-19 and MERS antigens via nanobody-functionalized organic electrochemical transistors , 2021, Nature Biomedical Engineering.

[7]  Christopher J. Tassone,et al.  Unraveling the Unconventional Order of a High-Mobility Indacenodithiophene-Benzothiadiazole Copolymer. , 2021, ACS macro letters.

[8]  Ian E. Jacobs,et al.  Charge transport physics of a unique class of rigid-rod conjugated polymers with fused-ring conjugated units linked by double carbon-carbon bonds , 2021, Science Advances.

[9]  H. Sirringhaus,et al.  The effect of the dielectric end groups on the positive bias stress stability of N2200 organic field effect transistors , 2021, APL Materials.

[10]  J. Viana,et al.  A Review on Materials and Technologies for Organic Large‐Area Electronics , 2021, Advanced Materials Technologies.

[11]  Shouke Yan,et al.  Oriented Conjugated Copolymer Films with Controlled Crystal Forms and Molecular Stacking Modes for Enhanced Charge Transport and Photoresponsivity , 2021 .

[12]  Jin-Hu Dou,et al.  Approaching Crystal Structure and High Electron Mobility in Conjugated Polymer Crystals , 2021, Advanced materials.

[13]  Ian E. Jacobs,et al.  Structural and Dynamic Disorder, Not Ionic Trapping, Controls Charge Transport in Highly Doped Conducting Polymers , 2021, Journal of the American Chemical Society.

[14]  H. Sirringhaus,et al.  Linking Glass‐Transition Behavior to Photophysical and Charge Transport Properties of High‐Mobility Conjugated Polymers , 2020, Advanced Functional Materials.

[15]  S. Inal,et al.  Organic Bioelectronics: From Functional Materials to Next‐Generation Devices and Power Sources , 2020, Advanced materials.

[16]  R. Friend,et al.  Stable Hexylphosphonate-Capped Blue-Emitting Quantum-Confined CsPbBr3 Nanoplatelets , 2020, ACS energy letters.

[17]  Satyaprasad P. Senanayak,et al.  Anisotropy of Charge Transport in a Uniaxially Aligned Fused Electron‐Deficient Polymer Processed by Solution Shear Coating , 2020, Advanced materials.

[18]  H. Sirringhaus,et al.  Charge transport in high-mobility conjugated polymers and molecular semiconductors , 2020, Nature Materials.

[19]  Jasmine P. H. Rivett,et al.  Chain Coupling and Luminescence in High-Mobility, Low Disorder Conjugated Polymers. , 2019, ACS nano.

[20]  X. Crispin,et al.  Interfaces in organic electronics , 2019, Nature Reviews Materials.

[21]  Johannes M. Richter,et al.  Short contacts between chains enhancing luminescence quantum yields and carrier mobilities in conjugated copolymers , 2019, Nature Communications.

[22]  George D. Spyropoulos,et al.  Internal ion-gated organic electrochemical transistor: A building block for integrated bioelectronics , 2019, Science Advances.

[23]  L. Torsi,et al.  Single-molecule detection with a millimetre-sized transistor , 2018, Nature Communications.

[24]  H. Sirringhaus,et al.  On the manifestation of electron-electron interactions in the thermoelectric response of semicrystalline conjugated polymers with low energetic disorder , 2018 .

[25]  H. Sirringhaus,et al.  Charge Mobility Enhancement for Conjugated DPP-Selenophene Polymer by Simply Replacing One Bulky Branching Alkyl Chain with Linear One at Each DPP Unit , 2018 .

[26]  Ian E. Jacobs,et al.  Put Your Backbone into It: Excited-State Structural Relaxation of PffBT4T-2DT Conducting Polymer in Solution , 2018 .

[27]  Joshua H. Carpenter,et al.  Integrated circuits based on conjugated polymer monolayer , 2018, Nature Communications.

[28]  D. Ginger,et al.  Correlating Photoluminescence Heterogeneity with Local Electronic Properties in Methylammonium Lead Tribromide Perovskite Thin Films , 2017 .

[29]  H. Sirringhaus,et al.  High operational and environmental stability of high-mobility conjugated polymer field-effect transistors through the use of molecular additives. , 2017, Nature materials.

[30]  Boris Murmann,et al.  Highly stretchable polymer semiconductor films through the nanoconfinement effect , 2017, Science.

[31]  I. McCulloch,et al.  Reduced voltage losses yield 10% efficient fullerene free organic solar cells with >1 V open circuit voltages† †Electronic supplementary information (ESI) available. See DOI: 10.1039/c6ee02598f Click here for additional data file. , 2016, Energy & environmental science.

[32]  Joshua H. Carpenter,et al.  Coulomb Enhanced Charge Transport in Semicrystalline Polymer Semiconductors , 2016 .

[33]  C. B. Nielsen,et al.  Azaisoindigo conjugated polymers for high performance n-type and ambipolar thin film transistor applications , 2016 .

[34]  C. McNeill,et al.  NEXAFS spectroscopy of conjugated polymers , 2016 .

[35]  H. Ade,et al.  Fast charge separation in a non-fullerene organic solar cell with a small driving force , 2016, Nature Energy.

[36]  X. Crispin,et al.  Experimental evidence that short-range intermolecular aggregation is sufficient for efficient charge transport in conjugated polymers , 2015, Proceedings of the National Academy of Sciences.

[37]  Sung-Jin Choi,et al.  Extraction of Propagation Delay-Correlated Mobility and Its Verification for Amorphous InGaZnO Thin-Film Transistor-Based Inverters , 2015, IEEE Transactions on Electron Devices.

[38]  Yuhang Liu,et al.  High-efficiency non-fullerene organic solar cells enabled by a difluorobenzothiadiazole-based donor polymer combined with a properly matched small molecule acceptor , 2015 .

[39]  He Yan,et al.  Aggregation and morphology control enables multiple cases of high-efficiency polymer solar cells , 2014, Nature Communications.

[40]  David Beljonne,et al.  Approaching disorder-free transport in high-mobility conjugated polymers , 2014, Nature.

[41]  K. Gmucová,et al.  Energy resolved electrochemical impedance spectroscopy for electronic structure mapping in organic semiconductors , 2014 .

[42]  John R. Reynolds,et al.  25th Anniversary Article: High‐Mobility Hole and Electron Transport Conjugated Polymers: How Structure Defines Function , 2014, Advanced materials.

[43]  H. Sirringhaus,et al.  Field-effect modulated Seebeck coefficient measurements in an organic polymer using a microfabricated on-chip architecture , 2014 .

[44]  M. Toney,et al.  A general relationship between disorder, aggregation and charge transport in conjugated polymers. , 2013, Nature materials.

[45]  H. Sirringhaus,et al.  Two-Dimensional Carrier Distribution in Top-Gate Polymer Field-Effect Transistors: Correlation between Width of Density of Localized States and Urbach Energy , 2013, Advanced materials.

[46]  Henning Sirringhaus,et al.  Molecular origin of high field-effect mobility in an indacenodithiophene–benzothiadiazole copolymer , 2013, Nature Communications.

[47]  Henning Sirringhaus,et al.  Microstructure of polycrystalline PBTTT films: domain mapping and structure formation. , 2012, ACS nano.

[48]  M. Kappl,et al.  Organic Field‐Effect Transistors based on Highly Ordered Single Polymer Fibers , 2012, Advanced materials.

[49]  H. Sirringhaus,et al.  Very Low Degree of Energetic Disorder as the Origin of High Mobility in an n‐channel Polymer Semiconductor , 2011 .

[50]  S. D. Hudson,et al.  In‐Plane Liquid Crystalline Texture of High‐Performance Thienothiophene Copolymer Thin Films , 2010 .

[51]  H. Sirringhaus,et al.  Conjugated‐Polymer‐Based Lateral Heterostructures Defined by High‐Resolution Photolithography , 2010 .

[52]  Alberto Salleo,et al.  Indacenodithiophene semiconducting polymers for high-performance, air-stable transistors. , 2010, Journal of the American Chemical Society.

[53]  F. Spano The spectral signatures of Frenkel polarons in H- and J-aggregates. , 2010, Accounts of chemical research.

[54]  A. Arias,et al.  Materials and applications for large area electronics: solution-based approaches. , 2010, Chemical reviews.

[55]  A. Facchetti,et al.  A high-mobility electron-transporting polymer for printed transistors , 2009, Nature.

[56]  Maxim Shkunov,et al.  Liquid-crystalline semiconducting polymers with high charge-carrier mobility , 2006, Nature materials.

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

[58]  Janos Veres,et al.  Low‐k Insulators as the Choice of Dielectrics in Organic Field‐Effect Transistors , 2003 .

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

[60]  D. Emin Enhanced Seebeck coefficient from carrier-induced vibrational softening , 1999 .

[61]  R. van Langevelde,et al.  Effect of gate-field dependent mobility degradation on distortion analysis in MOSFETs , 1997 .

[62]  S. L. Mayo,et al.  DREIDING: A generic force field for molecular simulations , 1990 .

[63]  A. F. Tasch,et al.  A universal MOSFET mobility degradation model for circuit simulation , 1990, IEEE Trans. Comput. Aided Des. Integr. Circuits Syst..

[64]  Warren Jackson,et al.  DIRECT MEASUREMENT OF GAP STATE ABSORPTION IN HYDROGENATED AMORPHOUS SILICON BY PHOTOTHERMAL DEFLECTION SPECTROSCOPY , 1982 .

[65]  A. Boccara,et al.  Photothermal deflection spectroscopy and detection. , 1981, Applied optics.

[66]  Henning Sirringhaus,et al.  Critical assessment of charge mobility extraction in FETs. , 2017, Nature materials.

[67]  Ashok Nedungadi,et al.  Design of linear CMOS transconductance elements , 1984 .

[68]  J. Gasteiger,et al.  ITERATIVE PARTIAL EQUALIZATION OF ORBITAL ELECTRONEGATIVITY – A RAPID ACCESS TO ATOMIC CHARGES , 1980 .