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Facile ab initio approach for self-localized polarons from canonical transformations

Lee, Nien-En and Chen, Hsiao-Yi and Zhou, Jin-Jian and Bernardi, Marco (2020) Facile ab initio approach for self-localized polarons from canonical transformations. . (Unpublished) https://resolver.caltech.edu/CaltechAUTHORS:20201203-151018693

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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 wavefunction 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.


Item Type:Report or Paper (Discussion Paper)
Related URLs:
URLURL TypeDescription
http://arxiv.org/abs/2011.03620arXivDiscussion Paper
ORCID:
AuthorORCID
Chen, Hsiao-Yi0000-0003-1962-5767
Zhou, Jin-Jian0000-0002-1182-9186
Bernardi, Marco0000-0001-7289-9666
Additional Information:This work was supported by the Air Force Office of Scientific Research through the Young Investigator Program, Grant FA9550-18-1-0280. J.-J. Z. was supported by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award No. DE-SC0004993. H.-Y. C. acknowledges support by the J. Yang Fellowship. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the US Department of Energy under Contract No. DE-AC02-05CH11231.
Group:JCAP
Funders:
Funding AgencyGrant Number
Air Force Office of Scientific Research (AFOSR)FA9550-18-1-0280
Department of Energy (DOE)DE-SC0004993
J. Yang Family and FoundationUNSPECIFIED
Department of Energy (DOE)DE-AC02-05CH11231
Record Number:CaltechAUTHORS:20201203-151018693
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20201203-151018693
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:106897
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:05 Dec 2020 01:56
Last Modified:05 Dec 2020 01:56

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