Structural and Dynamic Disorder, Not Ionic Trapping, Controls Charge Transport in Highly Doped Conducting Polymers

Jacobs, Ian E.; D’Avino, Gabriele; Lemaur, Vincent; Lin, Yue; Huang, Yuxuan; Chen, Chen; Harrelson, Thomas F.; Wood, William; Spalek, Leszek J.; Mustafa, Tarig; O’Keefe, Christopher A.; Ren, Xinglong; Simatos, Dimitrios; Tjhe, Dion; Statz, Martin; Strzalka, Joseph W.; Lee, Jin-Kyun; McCulloch, Iain; Fratini, Simone; Beljonne, David; Sirringhaus, Henning

doi:10.1021/jacs.1c10651

Title: Structural and Dynamic Disorder, Not Ionic Trapping, Controls Charge Transport in Highly Doped Conducting Polymers

Journal Article · 14 February 2022 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.1c10651 · OSTI ID:1869179

^[1];

^[2]; Lemaur, Vincent ^[3];

^[1]; Huang, Yuxuan ^[1]; Chen, Chen ^[1]; Harrelson, Thomas F. ^[4]; Wood, William ^[1]; Spalek, Leszek J. ^[1]; Mustafa, Tarig ^[1]; O’Keefe, Christopher A. ^[1]; Ren, Xinglong ^[1]; Simatos, Dimitrios ^[1]; Tjhe, Dion ^[1]; Statz, Martin ^[1];

^[5];

^[6];

^[7]; Fratini, Simone ^[2];

^[3] more »

Univ. of Cambridge (United Kingdom)
Univ. of Grenoble Alpes, Grenoble (France)
Univ. of Mons (Belgium)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)
Inha Univ., Incheon (South Korea)
Univ. of Oxford (United Kingdom); King Abdullah University of Science and Technology (KAUST), Thuwal (Saudi Arabia)

Doped organic semiconductors are critical to emerging device applications, including thermoelectrics, bioelectronics, and neuromorphic computing devices. It is commonly assumed that low conductivities in these materials result primarily from charge trapping by the Coulomb potentials of the dopant counter-ions. Here, we present a combined experimental and theoretical study rebutting this belief. Using a newly developed doping technique, we find the conductivity of several classes of high-mobility conjugated polymers to be strongly correlated with paracrystalline disorder but poorly correlated with ionic size, suggesting that Coulomb traps do not limit transport. A general model for interacting electrons in highly doped polymers is proposed and carefully parameterized against atomistic calculations, enabling the calculation of electrical conductivity within the framework of transient localisation theory. Theoretical calculations are in excellent agreement with experimental data, providing insights into the disordered-limited nature of charge transport and suggesting new strategies to further improve conductivities.

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Research Organization:: Argonne National Laboratory (ANL), Lemont, IL (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: Cambridge Commonwealth European and International Trust; Engineering and Physical Sciences Research Council (EPSRC); European Research Council (ERC); National Science Foundation (NSF); Royal Society Newton International Fellowship; USDOE Office of Science (SC); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357

OSTI ID:: 1869179

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 7 Vol. 144; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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