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Long-range quadrupole electron-phonon interaction from first principles

Park, Jinsoo and Zhou, Jin-Jian and Jhalani, Vatsal A. and Dreyer, Cyrus E. and Bernardi, Marco (2020) Long-range quadrupole electron-phonon interaction from first principles. Physical Review B, 102 (12). Art. No. 125203. ISSN 2469-9950. https://resolver.caltech.edu/CaltechAUTHORS:20200518-152636389

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Abstract

Lattice vibrations in materials induce perturbations on the electron dynamics in the form of long-range (dipole and quadrupole) and short-range (octopole and higher) potentials. The dipole Fröhlich term can be included in current first-principles electron-phonon (e-ph) calculations and is present only in polar materials. The quadrupole e-ph interaction is present in both polar and nonpolar materials, but currently it cannot be computed from first principles. Here we show an approach to compute the quadrupole e-ph interaction and include it in ab initio calculations of e-ph matrix elements. The accuracy of the approach is demonstrated by comparing with direct density functional perturbation theory calculations. We apply our method to silicon as a case of a nonpolar semiconductor and tetragonal PbTiO₃ as a case of a polar piezoelectric material. In both materials we find that the quadrupole term strongly impacts the e-ph matrix elements. Analysis of e-ph interactions for different phonon modes reveals that the quadrupole term mainly affects optical modes in silicon and acoustic modes in PbTiO₃, although the quadrupole term is needed for all modes to achieve quantitative accuracy. The effect of the quadrupole e-ph interaction on electron scattering processes and transport is shown to be important. Our approach enables accurate studies of e-ph interactions in broad classes of nonpolar, polar, and piezoelectric materials.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1103/PhysRevB.102.125203DOIArticle
https://arxiv.org/abs/2003.13782arXivDiscussion Paper
ORCID:
AuthorORCID
Park, Jinsoo0000-0002-1763-5788
Zhou, Jin-Jian0000-0002-1182-9186
Jhalani, Vatsal A.0000-0003-0866-0858
Bernardi, Marco0000-0001-7289-9666
Additional Information:© 2020 American Physical Society. Received 30 March 2020; accepted 29 May 2020; published 21 September 2020. J.P. acknowledges support by the Korea Foundation for Advanced Studies. V.A.J. thanks the Resnick Sustainability Institute at Caltech for fellowship support. This work was supported by the National Science Foundation under Grants No. DMR-1750613 for theory development and No. ACI-1642443 for code development. J.-J.Z. acknowledges partial support from the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, as follows: the development of some computational methods employed in this work was supported through the Office of Science of the US Department of Energy under Award No. DE-SC0004993. C.E.D. acknowledges support from the National Science Foundation under Grant No. DMR-1918455. The Flatiron Institute is a division of the Simons Foundation. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the US Department of Energy under Contract No. DE-AC02-05CH11231.
Group:JCAP, Resnick Sustainability Institute
Funders:
Funding AgencyGrant Number
Korea Foundation for Advanced StudiesUNSPECIFIED
Resnick Sustainability InstituteUNSPECIFIED
NSFDMR-1750613
NSFACI-1642443
Joint Center for Artificial Photosynthesis (JCAP)UNSPECIFIED
Department of Energy (DOE)DE-SC0004993
NSFDMR-1918455
Simons FoundationUNSPECIFIED
Department of Energy (DOE)DE-AC02-05CH11231
Issue or Number:12
Record Number:CaltechAUTHORS:20200518-152636389
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20200518-152636389
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:103291
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:18 May 2020 23:13
Last Modified:21 Sep 2020 22:30

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