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

Benjamin K. Chang1*, Jin-Jian Zhou1, Nien-En Lee1, Marco Bernardi1*

1 Department of Applied Physics and Materials Science, California Institute of Technology, Pasadena, California 91125, USA

* Corresponding authors emails: bkchang@caltech.edu, bmarco@caltech.edu
DOI10.24435/materialscloud:6t-e0 [version v2]

Publication date: Jan 12, 2022

How to cite this record

Benjamin K. Chang, Jin-Jian Zhou, Nien-En Lee, Marco Bernardi, Intermediate polaronic charge transport in organic crystals from a many-body first-principles approach, Materials Cloud Archive 2022.4 (2022), doi: 10.24435/materialscloud:6t-e0.


Predicting the electrical properties of organic molecular crystals (OMCs) is challenging due to their complex crystal structures and electron-phonon (e-ph) interactions. Charge transport in OMCs is conventionally categorized into two limiting regimes – band transport, characterized by weak 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 OMCs in the 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 100–300 K. Our analysis reveals that electrons couple strongly with both inter- and intramolecular phonons in the intermediate regime, as evidenced by the formation of a broad polaron satellite peak in the electron spectral function and the failure of the Boltzmann transport equation (BTE). Our study advances quantitative modeling of charge transport in complex organic crystals. This dataset contains input and output files required to reproduce the BTE results presented in our work.

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File name Size Description
134.0 MiB Collection of all files which were used to produce the BTE data of the paper: input files and output files.
3.5 KiB The README.txt file describes the content of the compressed file "naph_perturbo.tar.gz"


Files and data are licensed under the terms of the following license: Creative Commons Attribution 4.0 International.
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External references

Preprint (Preprint where the data is discussed)


organic crystal molecular crystal first-principles calculations naphthalene Boltzmann equation charge transport carrier mobility polaron electron-phonon coupling electron-phonon scattering rate

Version history:

2022.4 (version v2) [This version] Jan 12, 2022 DOI10.24435/materialscloud:6t-e0
2022.1 (version v1) Jan 11, 2022 DOI10.24435/materialscloud:s0-5q