Benjamin K. Chang^1*, Jin-Jian Zhou¹, Nien-En Lee¹, Marco Bernardi^1*

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:s0-5q [version v1]

Publication date: Jan 11, 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 2022.1 (2022), https://doi.org/10.24435/materialscloud:s0-5q

Description

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.

Materials Cloud sections using this data

Files

File name	Size	Description
naph-perturbo.tar.gz MD5md5:7b67f60f303cf3fbad06c3cc7ad5a2e7	133.7 MiB	Collection of all files which were used to produce the BTE data of the paper: input files and output files.
README.txt MD5md5:42bd6b2281440560cd90dd230503d9f3	2.8 KiB	The README.txt file describes the content of the compressed file "naph-perturbo.tar.gz"

License

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External references

Keywords

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