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Title: Ab initio electron-phonon interactions using atomic orbital wave functions

Abstract

The interaction among electrons and lattice vibrations determines key physical properties of materials, including their electrical and heat transport, excited electron dynamics, phase transitions, and superconductivity. We present an ab initio method that employs atomic orbital (AO) wave functions to compute the electron-phonon (e-ph) interactions in materials and interpolate the e-ph coupling matrix elements to fine Brillouin zone grids. We illustrate the numerical implementation of such AO-based e-ph calculations, and benchmark them against direct density functional theory calculations and Wannier function (WF) interpolation. The prime advantages of AOs over WFs for e-ph calculations are outlined. Since AOs are fixed basis functions associated with the atoms, they circumvent the need to generate a material-specific localized basis set with a trial-and-error approach, as is needed in WFs. Therefore, AOs are ideal to compute e-ph interactions in chemically and structurally complex materials for which WFs are challenging to generate, and are also promising for high-throughput materials discovery. Although our findings focus on AOs, the formalism we present generalizes e-ph calculations to arbitrary localized basis sets, with WFs recovered as a special case.

Authors:
 [1];  [1]
  1. California Inst. of Technology (CalTech), Pasadena, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC); National Science Foundation (NSF)
OSTI Identifier:
1544263
Alternate Identifier(s):
OSTI ID: 1457479
Grant/Contract Number:  
[ACI-1642443; ACI-1548562; AC02-05CH11231]
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
[ Journal Volume: 97; Journal Issue: 23]; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Agapito, Luis A., and Bernardi, Marco. Ab initio electron-phonon interactions using atomic orbital wave functions. United States: N. p., 2018. Web. doi:10.1103/PhysRevB.97.235146.
Agapito, Luis A., & Bernardi, Marco. Ab initio electron-phonon interactions using atomic orbital wave functions. United States. doi:10.1103/PhysRevB.97.235146.
Agapito, Luis A., and Bernardi, Marco. Wed . "Ab initio electron-phonon interactions using atomic orbital wave functions". United States. doi:10.1103/PhysRevB.97.235146. https://www.osti.gov/servlets/purl/1544263.
@article{osti_1544263,
title = {Ab initio electron-phonon interactions using atomic orbital wave functions},
author = {Agapito, Luis A. and Bernardi, Marco},
abstractNote = {The interaction among electrons and lattice vibrations determines key physical properties of materials, including their electrical and heat transport, excited electron dynamics, phase transitions, and superconductivity. We present an ab initio method that employs atomic orbital (AO) wave functions to compute the electron-phonon (e-ph) interactions in materials and interpolate the e-ph coupling matrix elements to fine Brillouin zone grids. We illustrate the numerical implementation of such AO-based e-ph calculations, and benchmark them against direct density functional theory calculations and Wannier function (WF) interpolation. The prime advantages of AOs over WFs for e-ph calculations are outlined. Since AOs are fixed basis functions associated with the atoms, they circumvent the need to generate a material-specific localized basis set with a trial-and-error approach, as is needed in WFs. Therefore, AOs are ideal to compute e-ph interactions in chemically and structurally complex materials for which WFs are challenging to generate, and are also promising for high-throughput materials discovery. Although our findings focus on AOs, the formalism we present generalizes e-ph calculations to arbitrary localized basis sets, with WFs recovered as a special case.},
doi = {10.1103/PhysRevB.97.235146},
journal = {Physical Review B},
number = [23],
volume = [97],
place = {United States},
year = {2018},
month = {6}
}

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