Intermediate polaronic charge transport in organic crystals from a many-body first-principles approach
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.
Document Details
- Document Type
- Pub Defense Publication
- Publication Date
- Apr 11, 2022
- Source ID
- 10.1038/s41524-022-00742-6
Entities
People
- Benjamin K. Chang
- Jin-Jian Zhou
- Marco Bernardi
- Nien-en Lee
Organizations
- Air Force Office of Scientific Research
- National Science Foundation
- United States Department of Energy