A Caltech Library Service

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 (2021) Facile ab initio approach for self-localized polarons from canonical transformations. Physical Review Materials, 5 (6). Art. No. 063805. ISSN 2475-9953. doi:10.1103/PhysRevMaterials.5.063805.

[img] PDF - Published Version
See Usage Policy.

[img] PDF - Submitted Version
See Usage Policy.


Use this Persistent URL to link to this item:


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.

Item Type:Article
Related URLs:
URLURL TypeDescription Paper
Lee, Nien-En0000-0002-3172-7750
Chen, Hsiao-Yi0000-0003-1962-5767
Zhou, Jin-Jian0000-0002-1182-9186
Bernardi, Marco0000-0001-7289-9666
Additional Information:© 2021 American Physical Society. Received 9 November 2020; revised 24 April 2021; accepted 8 June 2021; published 24 June 2021. This work was supported by the Air Force Office of Scientific Research through the Young Investigator Program, Grant No. 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 (NERSC), a U.S. Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under Contract No. DE-AC02-05CH11231.
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
Issue or Number:6
Record Number:CaltechAUTHORS:20201203-151018693
Persistent URL:
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:106897
Deposited By: George Porter
Deposited On:05 Dec 2020 01:56
Last Modified:11 Apr 2022 22:17

Repository Staff Only: item control page