Facile ab initio approach for self-localized polarons from canonical transformations
Abstract
Electronic states in a crystal can localize due to strong electron-phonon (e-ph) interactions, forming so-called small polarons. Methods to predict the formation and energetics of small polarons are either computationally costly or not geared toward quantitative predictions. Here we show a formalism based on canonical transformations to compute the polaron formation energy and wave function using ab initio e-ph interactions. Comparison of the calculated polaron and band-edge energies allows us to determine whether charge carriers in a material favor a localized small polaron over a delocalized Bloch state. Due to its low computational cost, our approach enables efficient studies of the formation and energetics of small polarons, as we demonstrate by investigating electron and hole polaron formation in alkali halides and metal oxides and peroxides. We outline refinements of our scheme and extensions to compute transport in the polaron hopping regime.
- Publication Date:
- Research Org.:
- California Institute of Technology (CalTech), Pasadena, CA (United States); Univ. of California, Oakland, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1850882
- Grant/Contract Number:
- SC0004993; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review Materials
- Additional Journal Information:
- Journal Volume: 5; Journal Issue: 6; Journal ID: ISSN 2475-9953
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Materials Science; Electron-phonon coupling; Polarons; Insulators; Semiconductor compounds; Density functional calculations; First-principles calculations
Citation Formats
Lee, Nien-En, Chen, Hsiao-Yi, Zhou, Jin-Jian, and Bernardi, Marco. Facile ab initio approach for self-localized polarons from canonical transformations. United States: N. p., 2021.
Web. doi:10.1103/physrevmaterials.5.063805.
Lee, Nien-En, Chen, Hsiao-Yi, Zhou, Jin-Jian, & Bernardi, Marco. Facile ab initio approach for self-localized polarons from canonical transformations. United States. https://doi.org/10.1103/physrevmaterials.5.063805
Lee, Nien-En, Chen, Hsiao-Yi, Zhou, Jin-Jian, and Bernardi, Marco. Thu .
"Facile ab initio approach for self-localized polarons from canonical transformations". United States. https://doi.org/10.1103/physrevmaterials.5.063805. https://www.osti.gov/servlets/purl/1850882.
@article{osti_1850882,
title = {Facile ab initio approach for self-localized polarons from canonical transformations},
author = {Lee, Nien-En and Chen, Hsiao-Yi and Zhou, Jin-Jian and Bernardi, Marco},
abstractNote = {Electronic states in a crystal can localize due to strong electron-phonon (e-ph) interactions, forming so-called small polarons. Methods to predict the formation and energetics of small polarons are either computationally costly or not geared toward quantitative predictions. Here we show a formalism based on canonical transformations to compute the polaron formation energy and wave function using ab initio e-ph interactions. Comparison of the calculated polaron and band-edge energies allows us to determine whether charge carriers in a material favor a localized small polaron over a delocalized Bloch state. Due to its low computational cost, our approach enables efficient studies of the formation and energetics of small polarons, as we demonstrate by investigating electron and hole polaron formation in alkali halides and metal oxides and peroxides. We outline refinements of our scheme and extensions to compute transport in the polaron hopping regime.},
doi = {10.1103/physrevmaterials.5.063805},
journal = {Physical Review Materials},
number = 6,
volume = 5,
place = {United States},
year = {Thu Jun 24 00:00:00 EDT 2021},
month = {Thu Jun 24 00:00:00 EDT 2021}
}
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