Unraveling the Unconventional Order of a High-Mobility Indacenodithiophene–Benzothiadiazole Copolymer

Camila Cendra; Luke Balhorn; Weimin Zhang; Kathryn O’Hara; Karsten Bruening; Christopher J. Tassone; Hans-Georg Steinrück; Mengning Liang; Michael F. Toney; Iain McCulloch; Michael L Chabinyc; Alberto Salleo; Christopher J. Takacs

doi:10.1021/acsmacrolett.1c00547

Unraveling the Unconventional Order of a High-Mobility Indacenodithiophene–Benzothiadiazole Copolymer

Camila Cendra, Luke Balhorn, Weimin Zhang, Kathryn O’Hara, Karsten Bruening, Christopher J. Tassone, Hans-Georg Steinrück, Mengning Liang, Michael F. Toney, Iain McCulloch, Michael L Chabinyc, Alberto Salleo, Christopher J. Takacs

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

21 Scopus citations

Abstract

A new class of donor–acceptor (D–A) copolymers found to produce high charge carrier mobilities competitive with amorphous silicon (>1 cm2 V–1 s–1) exhibit the puzzling microstructure of substantial local order, however lacking long-range order and crystallinity previously deemed necessary for achieving high mobility. Here, we demonstrate the application of low-dose transmission electron microscopy to image and quantify the nanoscale and mesoscale organization of an archetypal D–A copolymer across areas comparable to electronic devices (≈9 μm2). The local structure is spatially resolved by mapping the backbone (001) spacing reflection, revealing nanocrystallites of aligned polymer chains throughout nearly the entire film. Analysis of the nanoscale structure of its ordered domains suggests significant short- and medium-range order and preferential grain boundary orientations. Moreover, we provide insights into the rich, interconnected mesoscale organization of this new family of D–A copolymers by analysis of the local orientational spatial autocorrelations.

Original language	English (US)
Pages (from-to)	1306-1314
Number of pages	9
Journal	ACS Macro Letters
DOIs	https://doi.org/10.1021/acsmacrolett.1c00547
State	Published - Oct 5 2021

Bibliographical note

KAUST Repository Item: Exported on 2021-10-13
Acknowledgements: We thank Dr. Elizabeth Montabana, Dr. David Buschnell, and Dr. Dong-Hua Chen for technical assistance with the Tecnai F20 transmission electron microscope. We also thank Dr. Sébastien Boutet at the Linac Coherent Light Source (LCLS) for FEL beamline assistance. Work by C.C. and L.B. on image analysis was supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES) under Award DE-SC0020046. C.C. and A.S. also gratefully acknowledge financial support from the National Science Foundation Award # DMR 1808401. C.J.T., K.O., and M.L.C. also acknowledge financial support from the National Science Foundation Award # DMR 1436263. We also gratefully acknowledge the support of NVIDIA Corporation with the donation of the Titan V GPU used for this research. Some of this work was performed at the Stanford-SLAC Cryo-EM Facilities, supported by Stanford University, SLAC, and the National Institutes of Health S10 Instrumentation Programs. Measurements at Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, were supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. Use of the Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515.

ASJC Scopus subject areas

Inorganic Chemistry
Organic Chemistry
Materials Chemistry
Polymers and Plastics

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10.1021/acsmacrolett.1c00547

https://repository.kaust.edu.sa/bitstream/10754/669055/1/Preprintfile1.pdf

Cite this

Cendra, C., Balhorn, L., Zhang, W., O’Hara, K., Bruening, K., Tassone, C. J., Steinrück, H.-G., Liang, M., Toney, M. F., McCulloch, I., Chabinyc, M. L., Salleo, A., & Takacs, C. J. (2021). Unraveling the Unconventional Order of a High-Mobility Indacenodithiophene–Benzothiadiazole Copolymer. ACS Macro Letters, 1306-1314. https://doi.org/10.1021/acsmacrolett.1c00547

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abstract = "A new class of donor–acceptor (D–A) copolymers found to produce high charge carrier mobilities competitive with amorphous silicon (>1 cm2 V–1 s–1) exhibit the puzzling microstructure of substantial local order, however lacking long-range order and crystallinity previously deemed necessary for achieving high mobility. Here, we demonstrate the application of low-dose transmission electron microscopy to image and quantify the nanoscale and mesoscale organization of an archetypal D–A copolymer across areas comparable to electronic devices (≈9 μm2). The local structure is spatially resolved by mapping the backbone (001) spacing reflection, revealing nanocrystallites of aligned polymer chains throughout nearly the entire film. Analysis of the nanoscale structure of its ordered domains suggests significant short- and medium-range order and preferential grain boundary orientations. Moreover, we provide insights into the rich, interconnected mesoscale organization of this new family of D–A copolymers by analysis of the local orientational spatial autocorrelations.",

author = "Camila Cendra and Luke Balhorn and Weimin Zhang and Kathryn O{\textquoteright}Hara and Karsten Bruening and Tassone, {Christopher J.} and Hans-Georg Steinr{\"u}ck and Mengning Liang and Toney, {Michael F.} and Iain McCulloch and Chabinyc, {Michael L} and Alberto Salleo and Takacs, {Christopher J.}",

note = "KAUST Repository Item: Exported on 2021-10-13 Acknowledgements: We thank Dr. Elizabeth Montabana, Dr. David Buschnell, and Dr. Dong-Hua Chen for technical assistance with the Tecnai F20 transmission electron microscope. We also thank Dr. S{\'e}bastien Boutet at the Linac Coherent Light Source (LCLS) for FEL beamline assistance. Work by C.C. and L.B. on image analysis was supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES) under Award DE-SC0020046. C.C. and A.S. also gratefully acknowledge financial support from the National Science Foundation Award # DMR 1808401. C.J.T., K.O., and M.L.C. also acknowledge financial support from the National Science Foundation Award # DMR 1436263. We also gratefully acknowledge the support of NVIDIA Corporation with the donation of the Titan V GPU used for this research. Some of this work was performed at the Stanford-SLAC Cryo-EM Facilities, supported by Stanford University, SLAC, and the National Institutes of Health S10 Instrumentation Programs. Measurements at Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, were supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. Use of the Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515.",

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doi = "10.1021/acsmacrolett.1c00547",

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T1 - Unraveling the Unconventional Order of a High-Mobility Indacenodithiophene–Benzothiadiazole Copolymer

AU - Cendra, Camila

AU - Balhorn, Luke

AU - Zhang, Weimin

AU - O’Hara, Kathryn

AU - Bruening, Karsten

AU - Tassone, Christopher J.

AU - Steinrück, Hans-Georg

AU - Liang, Mengning

AU - Toney, Michael F.

AU - McCulloch, Iain

AU - Chabinyc, Michael L

AU - Salleo, Alberto

AU - Takacs, Christopher J.

N1 - KAUST Repository Item: Exported on 2021-10-13 Acknowledgements: We thank Dr. Elizabeth Montabana, Dr. David Buschnell, and Dr. Dong-Hua Chen for technical assistance with the Tecnai F20 transmission electron microscope. We also thank Dr. Sébastien Boutet at the Linac Coherent Light Source (LCLS) for FEL beamline assistance. Work by C.C. and L.B. on image analysis was supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES) under Award DE-SC0020046. C.C. and A.S. also gratefully acknowledge financial support from the National Science Foundation Award # DMR 1808401. C.J.T., K.O., and M.L.C. also acknowledge financial support from the National Science Foundation Award # DMR 1436263. We also gratefully acknowledge the support of NVIDIA Corporation with the donation of the Titan V GPU used for this research. Some of this work was performed at the Stanford-SLAC Cryo-EM Facilities, supported by Stanford University, SLAC, and the National Institutes of Health S10 Instrumentation Programs. Measurements at Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, were supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. Use of the Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515.

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N2 - A new class of donor–acceptor (D–A) copolymers found to produce high charge carrier mobilities competitive with amorphous silicon (>1 cm2 V–1 s–1) exhibit the puzzling microstructure of substantial local order, however lacking long-range order and crystallinity previously deemed necessary for achieving high mobility. Here, we demonstrate the application of low-dose transmission electron microscopy to image and quantify the nanoscale and mesoscale organization of an archetypal D–A copolymer across areas comparable to electronic devices (≈9 μm2). The local structure is spatially resolved by mapping the backbone (001) spacing reflection, revealing nanocrystallites of aligned polymer chains throughout nearly the entire film. Analysis of the nanoscale structure of its ordered domains suggests significant short- and medium-range order and preferential grain boundary orientations. Moreover, we provide insights into the rich, interconnected mesoscale organization of this new family of D–A copolymers by analysis of the local orientational spatial autocorrelations.

AB - A new class of donor–acceptor (D–A) copolymers found to produce high charge carrier mobilities competitive with amorphous silicon (>1 cm2 V–1 s–1) exhibit the puzzling microstructure of substantial local order, however lacking long-range order and crystallinity previously deemed necessary for achieving high mobility. Here, we demonstrate the application of low-dose transmission electron microscopy to image and quantify the nanoscale and mesoscale organization of an archetypal D–A copolymer across areas comparable to electronic devices (≈9 μm2). The local structure is spatially resolved by mapping the backbone (001) spacing reflection, revealing nanocrystallites of aligned polymer chains throughout nearly the entire film. Analysis of the nanoscale structure of its ordered domains suggests significant short- and medium-range order and preferential grain boundary orientations. Moreover, we provide insights into the rich, interconnected mesoscale organization of this new family of D–A copolymers by analysis of the local orientational spatial autocorrelations.

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UR - https://pubs.acs.org/doi/10.1021/acsmacrolett.1c00547

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DO - 10.1021/acsmacrolett.1c00547

M3 - Article

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SN - 2161-1653

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EP - 1314

JO - ACS Macro Letters

JF - ACS Macro Letters

ER -

Unraveling the Unconventional Order of a High-Mobility Indacenodithiophene–Benzothiadiazole Copolymer

Abstract

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