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

Journal Article · · Physical Review Materials
 [1];  [2];  [2];  [2]
  1. California Institute of Technology (CalTech), Pasadena, CA (United States); OSTI
  2. California Institute of Technology (CalTech), Pasadena, CA (United States)
+ Show Author Affiliations
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.
Research Organization:
California Institute of Technology (CalTech), Pasadena, CA (United States); University of California, Oakland, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC)
Grant/Contract Number:
SC0004993; AC02-05CH11231
OSTI ID:
1850882
Journal Information:
Physical Review Materials, Journal Name: Physical Review Materials Journal Issue: 6 Vol. 5; ISSN PRMHAR; ISSN 2475-9953
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

36 MATERIALS SCIENCE
Density functional calculations
Electron-phonon coupling
First-principles calculations
Insulators
Materials Science
Polarons
Semiconductor compounds