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Intermediate polaronic charge transport in organic crystals from a many-body first-principles approach

Chang, Benjamin K. and Zhou, Jin-Jian and Lee, Nien-En and Bernardi, Marco (2022) Intermediate polaronic charge transport in organic crystals from a many-body first-principles approach. npj Computational Materials, 8 . Art. No. 63. ISSN 2057-3960. doi:10.1038/s41524-022-00742-6.

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Charge transport in organic molecular crystals (OMCs) is conventionally categorized into two limiting regimes − band transport, characterized by weak electron-phonon (e-ph) interactions, and charge hopping due to localized polarons formed by strong e-ph interactions. However, between these two limiting cases there is a less well understood intermediate regime where polarons are present but transport does not occur via hopping. Here we show a many-body first-principles approach that can accurately predict the carrier mobility in this intermediate regime and shed light on its microscopic origin. Our approach combines a finite-temperature cumulant method to describe strong e-ph interactions with Green-Kubo transport calculations. We apply this parameter-free framework to naphthalene crystal, demonstrating electron mobility predictions within a factor of 1.5−2 of experiment between 100 and 300 K. Our analysis reveals the formation of a broad polaron satellite peak in the electron spectral function and the failure of the Boltzmann equation in the intermediate regime.

Item Type:Article
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URLURL TypeDescription Paper ItemCode
Chang, Benjamin K.0000-0003-1304-9324
Zhou, Jin-Jian0000-0002-1182-9186
Lee, Nien-En0000-0002-3172-7750
Bernardi, Marco0000-0001-7289-9666
Alternate Title:Intermediate Polaronic Charge Transport in Organic Crystals from First Principles
Additional Information:© 2022 The Author(s). Published in partnership with the Shanghai Institute of Ceramics of the Chinese Academy of Sciences. This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit Received 13 January 2022; Accepted 24 February 2022; Published 11 April 2022. This work was supported by the National Science Foundation under Grant No. DMR-1750613. J.-J.Z. acknowledges support from the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, as follows: the development of some computational methods employed in this work was supported through the Office of Science of the US Department of Energy under Award No. DE-SC0004993. N.-E.L. was supported by the Air Force Office of Scientific Research through the Young Investigator Program, Grant FA9550-18-1-0280. This research used resources of the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under Contract No. DE-AC02-05CH11231. Data availability: The data supporting the findings of this study, and in particular the files for the electron-phonon and BTE calculations, are available on Materials Cloud Archive with the identifier doi:10.24435/materialscloud:6t-e0. The authors are available to provide additional data and information upon reasonable request. Code availability: The PERTURBO code used in this work is an open source software, and can be downloaded at The BTE subroutines are included in the current release, and the CK subroutines will be included in a future release. Contributions: B.K.C. and M.B. conceived and designed the research. B.K.C. performed calculation and analysis. J.-J.Z. and N.-E.L. provided technical and theoretical support. M.B. supervised the entire research project. All authors discussed the results and contributed to the manuscript. The authors declare no competing interests.
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Air Force Office of Scientific Research (AFOSR)FA9550-18-1-0280
Department of Energy (DOE)DE-AC02-05CH11231
Subject Keywords:Computational methods; Molecular electronics; Physical chemistry; Semiconductors
Record Number:CaltechAUTHORS:20210716-222534684
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Official Citation:Chang, B.K., Zhou, JJ., Lee, NE. et al. Intermediate polaronic charge transport in organic crystals from a many-body first-principles approach. npj Comput Mater 8, 63 (2022).
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:109890
Deposited By: George Porter
Deposited On:16 Jul 2021 22:56
Last Modified:11 Apr 2022 22:14

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