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

Chang, Benjamin K.; Zhou, Jin-Jian; Lee, Nien-En; Bernardi, Marco

doi:10.1038/s41524-022-00742-6

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

Journal Article · 10 April 2022 · npj Computational Materials

DOI: https://doi.org/10.1038/s41524-022-00742-6 · OSTI ID:1862577

Chang, Benjamin K.; Zhou, Jin-Jian; Lee, Nien-En;

Abstract 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.

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Research Organization:: California Institute of Technology (CalTech), Pasadena, CA (United States); University of California, Oakland, CA (United States)

Sponsoring Organization:: Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF); USDOE; USDOE Office of Science (SC)

Grant/Contract Number:: AC02-05CH11231; SC0004993

OSTI ID:: 1862577

Journal Information:: npj Computational Materials, Journal Name: npj Computational Materials Journal Issue: 1 Vol. 8; ISSN 2057-3960

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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

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