High-throughput analysis of Fröhlich-type polaron models

Pedro Monteiro Campos de Melo; Joao C. de Abreu; Bogdan Guster; Matteo Giantomassi; Zeila Zanolli; Xavier Gonze; Matthieu Jean Verstraete

doi:10.1038/s41524-023-01083-8

High-throughput analysis of Fröhlich-type polaron models

Pedro Monteiro Campos de Melo^*
, Joao C. de Abreu
, Bogdan Guster
, Matteo Giantomassi
, Zeila Zanolli
, Xavier Gonze
, Matthieu Jean Verstraete

^*Corresponding author for this work

University of Liege
Université catholique de Louvain

Research output: Contribution to journal › Article › Academic › peer-review

Abstract

The electron–phonon interaction is central to condensed matter, e.g. through electrical resistance, superconductivity or the formation of polarons, and has a strong impact on observables such as band gaps or optical spectra. The most common framework for band energy corrections is the Fröhlich model, which often agrees qualitatively with experiments in polar materials, but has limits for complex cases. A generalized version includes anisotropic and degenerate electron bands, and multiple phonons. In this work, we identify trends and outliers for the Fröhlich models on 1260 materials. We test the limits of the Fröhlich models and their perturbative treatment, in particular the large polaron hypothesis. Among our extended dataset most materials host perturbative large polarons, but there are many instances that are non-perturbative and/or localize on distances of a few bond lengths. We find a variety of behaviors, and analyze extreme cases with huge zero-point renormalization using the first-principles Allen-Heine-Cardona approach.

Original language	English
Article number	147
Number of pages	13
Journal	npj Computational Materials
Volume	9
Issue number	1
DOIs	https://doi.org/10.1038/s41524-023-01083-8
Publication status	Published - 18 Aug 2023

Bibliographical note

Publisher Copyright:
© 2023, Springer Nature Limited.

Funding

This work has been supported by the Fonds de la Recherche Scientifique (FRS-FNRS Belgium) through the PdR Grant No. T.0103.19 - ALPS, and by the Federal government of Belgium through the EoS Project ID 40007525. ZZ and PMMCM acknowledge financial support by the Netherlands Sector Plan program 2019-2023 and the research program “Materials for the Quantum Age” (QuMAt, registration number 024.005.006), part of the Gravitation program of the Dutch Ministry of Education, Culture and Science (OCW). This project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No. 951786 - NOMAD CoE. Computational resources have been provided by the CISM/UCLouvain and the CECI funded by the FRS-FNRS Belgium under Grant No. 2.5020.11, as well as the Tier-1 supercomputer of the Fédération Wallonie-Bruxelles, funded by the Walloon Region under grant agreement No. 1117545. We acknowledge a PRACE award granting access to MareNostrum4 at Barcelona Supercomputing Center (BSC), Spain (OptoSpin project id. 2020225411). Moreover, we also acknowledge a PRACE Tier-1 award in the DECI-16 call for project REM-EPI on Archer and Archer2 EPCC in Edinburgh. This work was sponsored by NWO-Domain Science for the use of supercomputer facilities.

Funders	Funder number
CECI	2.5020.11
CISM
NWO-Domain
UCLouvain
Horizon 2020 Framework Programme	951786
Belgische Federale Overheidsdiensten	40007525, 024.005.006, 2019-2023
Waalse Gewest	2020225411, 1117545
Fonds De La Recherche Scientifique - FNRS
Fédération Wallonie-Bruxelles
Ministerie van onderwijs, cultuur en wetenschap

Keywords

polarons
First-principles calculations
high-throughput simulations

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s41524-023-01083-8Final published version, 1.83 MBLicence: CC BY

Cite this

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title = "High-throughput analysis of Fr{\"o}hlich-type polaron models",

abstract = "The electron{\textendash}phonon interaction is central to condensed matter, e.g. through electrical resistance, superconductivity or the formation of polarons, and has a strong impact on observables such as band gaps or optical spectra. The most common framework for band energy corrections is the Fr{\"o}hlich model, which often agrees qualitatively with experiments in polar materials, but has limits for complex cases. A generalized version includes anisotropic and degenerate electron bands, and multiple phonons. In this work, we identify trends and outliers for the Fr{\"o}hlich models on 1260 materials. We test the limits of the Fr{\"o}hlich models and their perturbative treatment, in particular the large polaron hypothesis. Among our extended dataset most materials host perturbative large polarons, but there are many instances that are non-perturbative and/or localize on distances of a few bond lengths. We find a variety of behaviors, and analyze extreme cases with huge zero-point renormalization using the first-principles Allen-Heine-Cardona approach.",

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AU - Guster, Bogdan

AU - Giantomassi, Matteo

AU - Zanolli, Zeila

AU - Gonze, Xavier

AU - Verstraete, Matthieu Jean

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High-throughput analysis of Fröhlich-type polaron models

Abstract

Bibliographical note

Funding

Keywords

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