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Title: Variational Excitations in Real Solids: Optical Gaps and Insights into Many-Body Perturbation Theory

Abstract

We present an approach to studying optical band gaps in real solids in which quantum Monte Carlo methods allow for the application of a rigorous variational principle to both ground and excited state wave functions. In tests that include small, medium, and large band gap materials, optical gaps are predicted with a mean absolute deviation of 3.5% against experiment, less than half the equivalent errors for typical many-body perturbation theories. The approach is designed to be insensitive to the choice of density functional, a property we exploit in order to provide insight into how far different functionals are from satisfying the assumptions of many-body perturbation theory. Here, we explore this question most deeply in the challenging case of ZnO, where we show that, although many commonly used functionals have shortcomings, there does exist a one-particle basis in which perturbation theory’s zeroth-order picture is sound. Insights of this nature should be useful in guiding the future application and improvement of these widely used techniques.

Authors:
 [1]; ORCiD logo [2]
  1. Univ. of California, Berkeley, CA (United States)
  2. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1543235
Alternate Identifier(s):
OSTI ID: 1546491
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 123; Journal Issue: 3; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Zhao, Luning, and Neuscamman, Eric. Variational Excitations in Real Solids: Optical Gaps and Insights into Many-Body Perturbation Theory. United States: N. p., 2019. Web. doi:10.1103/PhysRevLett.123.036402.
Zhao, Luning, & Neuscamman, Eric. Variational Excitations in Real Solids: Optical Gaps and Insights into Many-Body Perturbation Theory. United States. doi:10.1103/PhysRevLett.123.036402.
Zhao, Luning, and Neuscamman, Eric. Tue . "Variational Excitations in Real Solids: Optical Gaps and Insights into Many-Body Perturbation Theory". United States. doi:10.1103/PhysRevLett.123.036402.
@article{osti_1543235,
title = {Variational Excitations in Real Solids: Optical Gaps and Insights into Many-Body Perturbation Theory},
author = {Zhao, Luning and Neuscamman, Eric},
abstractNote = {We present an approach to studying optical band gaps in real solids in which quantum Monte Carlo methods allow for the application of a rigorous variational principle to both ground and excited state wave functions. In tests that include small, medium, and large band gap materials, optical gaps are predicted with a mean absolute deviation of 3.5% against experiment, less than half the equivalent errors for typical many-body perturbation theories. The approach is designed to be insensitive to the choice of density functional, a property we exploit in order to provide insight into how far different functionals are from satisfying the assumptions of many-body perturbation theory. Here, we explore this question most deeply in the challenging case of ZnO, where we show that, although many commonly used functionals have shortcomings, there does exist a one-particle basis in which perturbation theory’s zeroth-order picture is sound. Insights of this nature should be useful in guiding the future application and improvement of these widely used techniques.},
doi = {10.1103/PhysRevLett.123.036402},
journal = {Physical Review Letters},
number = 3,
volume = 123,
place = {United States},
year = {2019},
month = {7}
}

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