n-type charge transport in heavily p-doped polymers

Zhiming Liang; Hyun Ho Choi; Xuyi Luo; Tuo Liu; Ashkan Abtahi; Uma Shantini Ramasamy; J. Andrew Hitron; Kyle N. Baustert; Jacob L. Hempel; Alex M. Boehm; Armin Ansary; Douglas R. Strachan; Jianguo Mei; Chad Risko; Vitaly Podzorov; Kenneth R. Graham

doi:10.1038/s41563-020-00859-3

n-type charge transport in heavily p-doped polymers

Zhiming Liang, Hyun Ho Choi, Xuyi Luo, Tuo Liu, Ashkan Abtahi, Uma Shantini Ramasamy, J. Andrew Hitron, Kyle N. Baustert, Jacob L. Hempel, Alex M. Boehm, Armin Ansary, Douglas R. Strachan, Jianguo Mei, Chad Risko, Vitaly Podzorov, Kenneth R. Graham

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

59 Scopus citations

Abstract

It is commonly assumed that charge-carrier transport in doped π-conjugated polymers is dominated by one type of charge carrier, either holes or electrons, as determined by the chemistry of the dopant. Here, through Seebeck coefficient and Hall effect measurements, we show that mobile electrons contribute substantially to charge-carrier transport in π-conjugated polymers that are heavily p-doped with strong electron acceptors. Specifically, the Seebeck coefficient of several p-doped polymers changes sign from positive to negative as the concentration of the oxidizing agents FeCl₃ or NOBF₄ increase, and Hall effect measurements for the same p-doped polymers reveal that electrons become the dominant delocalized charge carriers. Ultraviolet and inverse photoelectron spectroscopy measurements show that doping with oxidizing agents results in elimination of the transport gap at high doping concentrations. This approach of heavy p-type doping is demonstrated to provide a promising route to high-performance n-type organic thermoelectric materials.

Original language	English
Pages (from-to)	518-524
Number of pages	7
Journal	Nature Materials
Volume	20
Issue number	4
DOIs	https://doi.org/10.1038/s41563-020-00859-3
State	Published - Apr 2021

Bibliographical note

Funding Information:
K.R.G., Z.L., T.L., A.M.B. and A. Abtahi. acknowledge the donors of the American Chemical Society Petroleum Research Fund for partial support of this research (grant no. 57619-DNI10). K.R.G., A. Abtahi., K.N.B. and C.R. acknowledge support from the National Science Foundation (DMR-1905734). U.S.R. and C.R. acknowledge partial support from the Office of Naval Research Young Investigator Program (N00014-18-1-2448). J.L.H. and A. Ansary. were supported through the United States Department of Energy (0000223282) for performance of the low-temperature electrical conductivity measurements. Supercomputing resources on the Lipscomb High-Performance Supercomputing Cluster were provided by the Information Technology Services and the Center for Computational Sciences at the University of Kentucky. V.P. and H.H.C. acknowledge support from the National Science Foundation (ECCS-1806363). H.H.C. acknowledges partial support from the Center for Advanced Soft Electronics at Pohang University, which is funded by the Ministry of Science, ICT and Future Planning of the Republic of Korea as a Global Frontier Project (CASE-2011-0031628). J.M. and X.L. appreciate the support from the National Science Foundation (CAREER award no. 1653909).

Publisher Copyright:
© 2021, The Author(s), under exclusive licence to Springer Nature Limited.

ASJC Scopus subject areas

Chemistry (all)
Materials Science (all)
Condensed Matter Physics
Mechanics of Materials
Mechanical Engineering

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10.1038/s41563-020-00859-3

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title = "n-type charge transport in heavily p-doped polymers",

abstract = "It is commonly assumed that charge-carrier transport in doped π-conjugated polymers is dominated by one type of charge carrier, either holes or electrons, as determined by the chemistry of the dopant. Here, through Seebeck coefficient and Hall effect measurements, we show that mobile electrons contribute substantially to charge-carrier transport in π-conjugated polymers that are heavily p-doped with strong electron acceptors. Specifically, the Seebeck coefficient of several p-doped polymers changes sign from positive to negative as the concentration of the oxidizing agents FeCl3 or NOBF4 increase, and Hall effect measurements for the same p-doped polymers reveal that electrons become the dominant delocalized charge carriers. Ultraviolet and inverse photoelectron spectroscopy measurements show that doping with oxidizing agents results in elimination of the transport gap at high doping concentrations. This approach of heavy p-type doping is demonstrated to provide a promising route to high-performance n-type organic thermoelectric materials.",

author = "Zhiming Liang and Choi, {Hyun Ho} and Xuyi Luo and Tuo Liu and Ashkan Abtahi and Ramasamy, {Uma Shantini} and Hitron, {J. Andrew} and Baustert, {Kyle N.} and Hempel, {Jacob L.} and Boehm, {Alex M.} and Armin Ansary and Strachan, {Douglas R.} and Jianguo Mei and Chad Risko and Vitaly Podzorov and Graham, {Kenneth R.}",

note = "Funding Information: K.R.G., Z.L., T.L., A.M.B. and A. Abtahi. acknowledge the donors of the American Chemical Society Petroleum Research Fund for partial support of this research (grant no. 57619-DNI10). K.R.G., A. Abtahi., K.N.B. and C.R. acknowledge support from the National Science Foundation (DMR-1905734). U.S.R. and C.R. acknowledge partial support from the Office of Naval Research Young Investigator Program (N00014-18-1-2448). J.L.H. and A. Ansary. were supported through the United States Department of Energy (0000223282) for performance of the low-temperature electrical conductivity measurements. Supercomputing resources on the Lipscomb High-Performance Supercomputing Cluster were provided by the Information Technology Services and the Center for Computational Sciences at the University of Kentucky. V.P. and H.H.C. acknowledge support from the National Science Foundation (ECCS-1806363). H.H.C. acknowledges partial support from the Center for Advanced Soft Electronics at Pohang University, which is funded by the Ministry of Science, ICT and Future Planning of the Republic of Korea as a Global Frontier Project (CASE-2011-0031628). J.M. and X.L. appreciate the support from the National Science Foundation (CAREER award no. 1653909). Publisher Copyright: {\textcopyright} 2021, The Author(s), under exclusive licence to Springer Nature Limited.",

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AU - Choi, Hyun Ho

AU - Luo, Xuyi

AU - Liu, Tuo

AU - Abtahi, Ashkan

AU - Ramasamy, Uma Shantini

AU - Hitron, J. Andrew

AU - Baustert, Kyle N.

AU - Hempel, Jacob L.

AU - Boehm, Alex M.

AU - Ansary, Armin

AU - Strachan, Douglas R.

AU - Mei, Jianguo

AU - Risko, Chad

AU - Podzorov, Vitaly

AU - Graham, Kenneth R.

N1 - Funding Information: K.R.G., Z.L., T.L., A.M.B. and A. Abtahi. acknowledge the donors of the American Chemical Society Petroleum Research Fund for partial support of this research (grant no. 57619-DNI10). K.R.G., A. Abtahi., K.N.B. and C.R. acknowledge support from the National Science Foundation (DMR-1905734). U.S.R. and C.R. acknowledge partial support from the Office of Naval Research Young Investigator Program (N00014-18-1-2448). J.L.H. and A. Ansary. were supported through the United States Department of Energy (0000223282) for performance of the low-temperature electrical conductivity measurements. Supercomputing resources on the Lipscomb High-Performance Supercomputing Cluster were provided by the Information Technology Services and the Center for Computational Sciences at the University of Kentucky. V.P. and H.H.C. acknowledge support from the National Science Foundation (ECCS-1806363). H.H.C. acknowledges partial support from the Center for Advanced Soft Electronics at Pohang University, which is funded by the Ministry of Science, ICT and Future Planning of the Republic of Korea as a Global Frontier Project (CASE-2011-0031628). J.M. and X.L. appreciate the support from the National Science Foundation (CAREER award no. 1653909). Publisher Copyright: © 2021, The Author(s), under exclusive licence to Springer Nature Limited.

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N2 - It is commonly assumed that charge-carrier transport in doped π-conjugated polymers is dominated by one type of charge carrier, either holes or electrons, as determined by the chemistry of the dopant. Here, through Seebeck coefficient and Hall effect measurements, we show that mobile electrons contribute substantially to charge-carrier transport in π-conjugated polymers that are heavily p-doped with strong electron acceptors. Specifically, the Seebeck coefficient of several p-doped polymers changes sign from positive to negative as the concentration of the oxidizing agents FeCl3 or NOBF4 increase, and Hall effect measurements for the same p-doped polymers reveal that electrons become the dominant delocalized charge carriers. Ultraviolet and inverse photoelectron spectroscopy measurements show that doping with oxidizing agents results in elimination of the transport gap at high doping concentrations. This approach of heavy p-type doping is demonstrated to provide a promising route to high-performance n-type organic thermoelectric materials.

AB - It is commonly assumed that charge-carrier transport in doped π-conjugated polymers is dominated by one type of charge carrier, either holes or electrons, as determined by the chemistry of the dopant. Here, through Seebeck coefficient and Hall effect measurements, we show that mobile electrons contribute substantially to charge-carrier transport in π-conjugated polymers that are heavily p-doped with strong electron acceptors. Specifically, the Seebeck coefficient of several p-doped polymers changes sign from positive to negative as the concentration of the oxidizing agents FeCl3 or NOBF4 increase, and Hall effect measurements for the same p-doped polymers reveal that electrons become the dominant delocalized charge carriers. Ultraviolet and inverse photoelectron spectroscopy measurements show that doping with oxidizing agents results in elimination of the transport gap at high doping concentrations. This approach of heavy p-type doping is demonstrated to provide a promising route to high-performance n-type organic thermoelectric materials.

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ER -

n-type charge transport in heavily p-doped polymers

Abstract

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