Coulomb Enhanced Charge Transport in Semicrystalline Polymer Semiconductors

Riccardo Di Pietro; Iyad Nasrallah; Joshua Carpenter; Eliot Gann; Lisa Sophie Kölln; Lars Thomsen; Deepak Venkateshvaran; Kathryn O'Hara; Aditya Sadhanala; Michael Chabinyc; Christopher R. McNeill; Antonio Facchetti; Harald Ade; Henning Sirringhaus; Dieter Neher

doi:10.1002/adfm.201602080

Coulomb Enhanced Charge Transport in Semicrystalline Polymer Semiconductors

Riccardo Di Pietro^*, Iyad Nasrallah, Joshua Carpenter, Eliot Gann, Lisa Sophie Kölln, Lars Thomsen, Deepak Venkateshvaran, Kathryn O'Hara, Aditya Sadhanala, Michael Chabinyc, Christopher R. McNeill, Antonio Facchetti, Harald Ade, Henning Sirringhaus, Dieter Neher

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

26 Scopus citations

Abstract

Polymer semiconductors provide unique possibilities and flexibility in tailoring their optoelectronic properties to match specific application demands. The recent development of semicrystalline polymers with strongly improved charge transport properties forces a review of the current understanding of the charge transport mechanisms and how they relate to the polymer's chemical and structural properties. Here, the charge density dependence of field effect mobility in semicrystalline polymer semiconductors is studied. A simultaneous increase in mobility and its charge density dependence, directly correlated to the increase in average crystallite size of the polymer film, is observed. Further evidence from charge accumulation spectroscopy shows that charges accumulate in the crystalline regions of the polymer film and that the increase in crystallite size affects the average electronic orbitals delocalization. These results clearly point to an effect that is not caused by energetic disorder. It is instead shown that the inclusion of short range coulomb repulsion between charge carriers on nanoscale crystalline domains allows describing the observed mobility dependence in agreement with the structural and optical characterization. The conclusions that are extracted extend beyond pure transistor characterization and can provide new insights into charge carrier transport for regimes and timescales that are relevant to other optoelectronic devices.

Original language	English (US)
Pages (from-to)	8011-8022
Number of pages	12
Journal	Advanced Functional Materials
Volume	26
Issue number	44
DOIs	https://doi.org/10.1002/adfm.201602080
State	Published - Nov 22 2016

Funding

R.D.P. would like to thank Dr. Ilja Lange and Prof. Neil Greenham for helpful discussions while developing the theoretical model, Mr. Andreas Pucher and Mr. Patrick Panow for designing and fabricating the sample holder for the CAS setup used in Potsdam. X-ray characterization and analysis by NCSU was supported by NSF (DMR-1207032). J.C. was partially supported by a GAANN Fellowship. X-ray data were acquired at beamline 7.3.3 at the Advanced Light Source, which is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. Parts of this research were carried out on the soft X-ray and SAXS/WAXS beamlines at the Australian Synchrotron. C.R.M. acknowledges the support from the Australian Research Council (FT100100275, DP130102616). K.O. and M.L.C. were supported by NSF DMR-1207549. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. R.D.P. acknowledges the ERC sinergy grant SC2 for funding.

Keywords

charge transport
field-effect transistors
organic semiconductors
semicrystalline polymers

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
Condensed Matter Physics
General Chemistry
General Materials Science
Electrochemistry
Biomaterials

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Di Pietro, R., Nasrallah, I., Carpenter, J., Gann, E., Kölln, L. S., Thomsen, L., Venkateshvaran, D., O'Hara, K., Sadhanala, A., Chabinyc, M., McNeill, C. R., Facchetti, A., Ade, H., Sirringhaus, H., & Neher, D. (2016). Coulomb Enhanced Charge Transport in Semicrystalline Polymer Semiconductors. Advanced Functional Materials, 26(44), 8011-8022. https://doi.org/10.1002/adfm.201602080

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title = "Coulomb Enhanced Charge Transport in Semicrystalline Polymer Semiconductors",

abstract = "Polymer semiconductors provide unique possibilities and flexibility in tailoring their optoelectronic properties to match specific application demands. The recent development of semicrystalline polymers with strongly improved charge transport properties forces a review of the current understanding of the charge transport mechanisms and how they relate to the polymer's chemical and structural properties. Here, the charge density dependence of field effect mobility in semicrystalline polymer semiconductors is studied. A simultaneous increase in mobility and its charge density dependence, directly correlated to the increase in average crystallite size of the polymer film, is observed. Further evidence from charge accumulation spectroscopy shows that charges accumulate in the crystalline regions of the polymer film and that the increase in crystallite size affects the average electronic orbitals delocalization. These results clearly point to an effect that is not caused by energetic disorder. It is instead shown that the inclusion of short range coulomb repulsion between charge carriers on nanoscale crystalline domains allows describing the observed mobility dependence in agreement with the structural and optical characterization. The conclusions that are extracted extend beyond pure transistor characterization and can provide new insights into charge carrier transport for regimes and timescales that are relevant to other optoelectronic devices.",

keywords = "charge transport, field-effect transistors, organic semiconductors, semicrystalline polymers",

author = "{Di Pietro}, Riccardo and Iyad Nasrallah and Joshua Carpenter and Eliot Gann and K{\"o}lln, {Lisa Sophie} and Lars Thomsen and Deepak Venkateshvaran and Kathryn O'Hara and Aditya Sadhanala and Michael Chabinyc and McNeill, {Christopher R.} and Antonio Facchetti and Harald Ade and Henning Sirringhaus and Dieter Neher",

note = "Funding Information: R.D.P. would like to thank Dr. Ilja Lange and Prof. Neil Greenham for helpful discussions while developing the theoretical model, Mr. Andreas Pucher and Mr. Patrick Panow for designing and fabricating the sample holder for the CAS setup used in Potsdam. X-ray characterization and analysis by NCSU was supported by NSF (DMR-1207032). J.C. was partially supported by a GAANN Fellowship. X-ray data were acquired at beamline 7.3.3 at the Advanced Light Source, which is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. Parts of this research were carried out on the soft X-ray and SAXS/WAXS beamlines at the Australian Synchrotron. C.R.M. acknowledges the support from the Australian Research Council (FT100100275, DP130102616). K.O. and M.L.C. were supported by NSF DMR-1207549. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. R.D.P. acknowledges the ERC sinergy grant SC2 for funding. Publisher Copyright: {\textcopyright} 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim",

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month = nov,

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doi = "10.1002/adfm.201602080",

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Di Pietro, R, Nasrallah, I, Carpenter, J, Gann, E, Kölln, LS, Thomsen, L, Venkateshvaran, D, O'Hara, K, Sadhanala, A, Chabinyc, M, McNeill, CR, Facchetti, A, Ade, H, Sirringhaus, H & Neher, D 2016, 'Coulomb Enhanced Charge Transport in Semicrystalline Polymer Semiconductors', Advanced Functional Materials, vol. 26, no. 44, pp. 8011-8022. https://doi.org/10.1002/adfm.201602080

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T1 - Coulomb Enhanced Charge Transport in Semicrystalline Polymer Semiconductors

AU - Di Pietro, Riccardo

AU - Nasrallah, Iyad

AU - Carpenter, Joshua

AU - Gann, Eliot

AU - Kölln, Lisa Sophie

AU - Thomsen, Lars

AU - Venkateshvaran, Deepak

AU - O'Hara, Kathryn

AU - Sadhanala, Aditya

AU - Chabinyc, Michael

AU - McNeill, Christopher R.

AU - Facchetti, Antonio

AU - Ade, Harald

AU - Sirringhaus, Henning

AU - Neher, Dieter

N1 - Funding Information: R.D.P. would like to thank Dr. Ilja Lange and Prof. Neil Greenham for helpful discussions while developing the theoretical model, Mr. Andreas Pucher and Mr. Patrick Panow for designing and fabricating the sample holder for the CAS setup used in Potsdam. X-ray characterization and analysis by NCSU was supported by NSF (DMR-1207032). J.C. was partially supported by a GAANN Fellowship. X-ray data were acquired at beamline 7.3.3 at the Advanced Light Source, which is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. Parts of this research were carried out on the soft X-ray and SAXS/WAXS beamlines at the Australian Synchrotron. C.R.M. acknowledges the support from the Australian Research Council (FT100100275, DP130102616). K.O. and M.L.C. were supported by NSF DMR-1207549. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. R.D.P. acknowledges the ERC sinergy grant SC2 for funding. Publisher Copyright: © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

PY - 2016/11/22

Y1 - 2016/11/22

N2 - Polymer semiconductors provide unique possibilities and flexibility in tailoring their optoelectronic properties to match specific application demands. The recent development of semicrystalline polymers with strongly improved charge transport properties forces a review of the current understanding of the charge transport mechanisms and how they relate to the polymer's chemical and structural properties. Here, the charge density dependence of field effect mobility in semicrystalline polymer semiconductors is studied. A simultaneous increase in mobility and its charge density dependence, directly correlated to the increase in average crystallite size of the polymer film, is observed. Further evidence from charge accumulation spectroscopy shows that charges accumulate in the crystalline regions of the polymer film and that the increase in crystallite size affects the average electronic orbitals delocalization. These results clearly point to an effect that is not caused by energetic disorder. It is instead shown that the inclusion of short range coulomb repulsion between charge carriers on nanoscale crystalline domains allows describing the observed mobility dependence in agreement with the structural and optical characterization. The conclusions that are extracted extend beyond pure transistor characterization and can provide new insights into charge carrier transport for regimes and timescales that are relevant to other optoelectronic devices.

AB - Polymer semiconductors provide unique possibilities and flexibility in tailoring their optoelectronic properties to match specific application demands. The recent development of semicrystalline polymers with strongly improved charge transport properties forces a review of the current understanding of the charge transport mechanisms and how they relate to the polymer's chemical and structural properties. Here, the charge density dependence of field effect mobility in semicrystalline polymer semiconductors is studied. A simultaneous increase in mobility and its charge density dependence, directly correlated to the increase in average crystallite size of the polymer film, is observed. Further evidence from charge accumulation spectroscopy shows that charges accumulate in the crystalline regions of the polymer film and that the increase in crystallite size affects the average electronic orbitals delocalization. These results clearly point to an effect that is not caused by energetic disorder. It is instead shown that the inclusion of short range coulomb repulsion between charge carriers on nanoscale crystalline domains allows describing the observed mobility dependence in agreement with the structural and optical characterization. The conclusions that are extracted extend beyond pure transistor characterization and can provide new insights into charge carrier transport for regimes and timescales that are relevant to other optoelectronic devices.

KW - charge transport

KW - field-effect transistors

KW - organic semiconductors

KW - semicrystalline polymers

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ER -

Coulomb Enhanced Charge Transport in Semicrystalline Polymer Semiconductors

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