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Title: Effect of the electronic charge gap on LO bond-stretching phonons in undoped La2CuO4 calculated using LDA + U

Abstract

Typical density-functional theory calculations that wrongly predict undoped cuprates to be metallic also predict Cu-O half- and full-breathing phonon energies that are significantly softer than observed, presumably because of weak on-site Coulomb repulsion on the Cu 3d orbitals. We used DFT+U calculations with antiferromagnetic supercells of La2CuO4 to establish correlation between the on-site repulsion strength, tuned via adjusting the value of U, and phonon dispersions. We find that breathing and half-breathing phonons reach experimental values when U is tuned to obtain the correct optical gap and magnetic moments. We demonstrate that using distorted supercells within DFT+U is a promising framework to model phonons in undoped cuprates and other perovskite oxides with complex, interrelated structural and electronic degrees of freedom.

Authors:
ORCiD logo [1];  [1]
  1. Univ. of Colorado, Boulder, CO (United States)
Publication Date:
Research Org.:
Univ. of Colorado, Boulder, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1834320
Alternate Identifier(s):
OSTI ID: 1829750; OSTI ID: 1842470
Grant/Contract Number:  
SC0006939
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 104; Journal Issue: 13; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; phonons; correlated electrons; density functional theory; antiferromagnetism; cuprates; band gap; electron-phonon coupling; first-principles calculations; optical phonons; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Sterling, Tyler C., and Reznik, Dmitry. Effect of the electronic charge gap on LO bond-stretching phonons in undoped La2CuO4 calculated using LDA + U. United States: N. p., 2021. Web. doi:10.1103/physrevb.104.134311.
Sterling, Tyler C., & Reznik, Dmitry. Effect of the electronic charge gap on LO bond-stretching phonons in undoped La2CuO4 calculated using LDA + U. United States. https://doi.org/10.1103/physrevb.104.134311
Sterling, Tyler C., and Reznik, Dmitry. Mon . "Effect of the electronic charge gap on LO bond-stretching phonons in undoped La2CuO4 calculated using LDA + U". United States. https://doi.org/10.1103/physrevb.104.134311. https://www.osti.gov/servlets/purl/1834320.
@article{osti_1834320,
title = {Effect of the electronic charge gap on LO bond-stretching phonons in undoped La2CuO4 calculated using LDA + U},
author = {Sterling, Tyler C. and Reznik, Dmitry},
abstractNote = {Typical density-functional theory calculations that wrongly predict undoped cuprates to be metallic also predict Cu-O half- and full-breathing phonon energies that are significantly softer than observed, presumably because of weak on-site Coulomb repulsion on the Cu 3d orbitals. We used DFT+U calculations with antiferromagnetic supercells of La2CuO4 to establish correlation between the on-site repulsion strength, tuned via adjusting the value of U, and phonon dispersions. We find that breathing and half-breathing phonons reach experimental values when U is tuned to obtain the correct optical gap and magnetic moments. We demonstrate that using distorted supercells within DFT+U is a promising framework to model phonons in undoped cuprates and other perovskite oxides with complex, interrelated structural and electronic degrees of freedom.},
doi = {10.1103/physrevb.104.134311},
journal = {Physical Review B},
number = 13,
volume = 104,
place = {United States},
year = {Mon Oct 25 00:00:00 EDT 2021},
month = {Mon Oct 25 00:00:00 EDT 2021}
}

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