Comparison of the canonical transformation and energy functional formalisms for ab initio calculations of self-localized polarons

Luo, Yao; Chang, Benjamin K.; Bernardi, Marco

doi:10.1103/physrevb.105.155132

Comparison of the canonical transformation and energy functional formalisms for ab initio calculations of self-localized polarons

Journal Article · Tue Apr 19 04:00:00 EDT 2022 · Physical Review. B

DOI:https://doi.org/10.1103/physrevb.105.155132· OSTI ID:1979746

Luo, Yao ^[1]; Chang, Benjamin K. ^[2]; ^[2]

California Institute of Technology (CalTech), Pasadena, CA (United States); OSTI
California Institute of Technology (CalTech), Pasadena, CA (United States)

In materials with strong electron-phonon (e-ph) interactions, charge carriers can distort the surrounding lattice and become trapped, forming self-localized (small) polarons. We recently developed an ab initio approach based on canonical transformations to efficiently compute the formation and energetics of small polarons A different approach based on a Landau-Pekar energy functional has been proposed in the recent literature. Here in this work, we analyze and compare these two methods in detail. We show that the small polaron energy is identical in the two formalisms when using the same polaron wave function. We also show that our canonical transformation formalism can predict polaron band structures and can properly treat zero- and finite-temperature lattice vibration effects, although at present using a fixed polaron wave function. Conversely, the energy functional approach can compute the polaron wave function, but as we show here, it neglects lattice vibrations and cannot address polaron self-localization and thermal band narrowing. Taken together, this work relates two different methods developed recently to study polarons from first-principles, highlighting their merits and shortcomings and discussing them both in a unified formalism.

View Accepted Manuscript (DOE)

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), Basic Energy Sciences (BES); Air Force Office of Scientific Research (AFOSR); Liquid Sunlight Alliance

Grant/Contract Number:: SC0021266; SC0022088; AC02-05CH11231

OSTI ID:: 1979746

Journal Information:: Physical Review. B, Journal Name: Physical Review. B Journal Issue: 15 Vol. 105; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Comparison of the canonical transformation and energy functional formalisms for ab initio calculations of self-localized polarons

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