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Title: Electronic band structures and excitonic properties of delafossites: A $GW$-BSE study

Abstract

We report the band structures and excitonic properties of delafossites CuMO2 (M=Al, Ga, In, Sc, Y, Cr) calculated using the state-of-the-art GW-BSE approach. We evaluate different levels of self-consistency of the GW approximations, namely G0W0, GW0, GW, and QSGW, on the band structures and find that GW0, in general, predicts the band gaps in better agreement with experiments considering the electron-hole effect. For CuCrO2, the HSE wave function is used as the starting point for the perturbative GW0 calculations, since it corrects the band orders wrongly predicted by PBE. The discrepancy about the valence band characters of CuCrO2 is classified based on both HSE and QSGW calculations. The PBE wave functions, already good, are used for other delafossites. All the delafossites are shown to be indirect band gap semiconductors with large exciton binding energies, varying from 0.24 to 0.44 eV, in consistent with experimental findings. The excitation mechanisms are explained by examining the exciton amplitude projections on the band structures. Discrepancies compared with experiments are also addressed. The lowest and strongest exciton, mainly contributed from either Cu 3d → Cu 3p (Al, Ga, In) or Cu 3d → M 3d (M = Sc, Y, Cr) transitions, is always located atmore » the L point of the rhombohedral Brillouin zone.« less

Authors:
 [1]; ORCiD logo [1];  [1]
  1. Univ. of Toledo, OH (United States). Wright Center for Photovoltaics Innovation and Commercialization (PVIC), Dept. of Physics and Astronomy
Publication Date:
Research Org.:
Duke Univ., Durham, NC (United States); Univ. of California, Oakland, CA (United States). The Regents
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC)
OSTI Identifier:
1473869
Alternate Identifier(s):
OSTI ID: 1376917
Grant/Contract Number:  
EE0006712; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Applied Physics
Additional Journal Information:
Journal Volume: 122; Journal Issue: 8; Journal ID: ISSN 0021-8979
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats

Wang, Xiaoming, Meng, Weiwei, and Yan, Yanfa. Electronic band structures and excitonic properties of delafossites: A $GW$-BSE study. United States: N. p., 2017. Web. https://doi.org/10.1063/1.4991913.
Wang, Xiaoming, Meng, Weiwei, & Yan, Yanfa. Electronic band structures and excitonic properties of delafossites: A $GW$-BSE study. United States. https://doi.org/10.1063/1.4991913
Wang, Xiaoming, Meng, Weiwei, and Yan, Yanfa. Fri . "Electronic band structures and excitonic properties of delafossites: A $GW$-BSE study". United States. https://doi.org/10.1063/1.4991913. https://www.osti.gov/servlets/purl/1473869.
@article{osti_1473869,
title = {Electronic band structures and excitonic properties of delafossites: A $GW$-BSE study},
author = {Wang, Xiaoming and Meng, Weiwei and Yan, Yanfa},
abstractNote = {We report the band structures and excitonic properties of delafossites CuMO2 (M=Al, Ga, In, Sc, Y, Cr) calculated using the state-of-the-art GW-BSE approach. We evaluate different levels of self-consistency of the GW approximations, namely G0W0, GW0, GW, and QSGW, on the band structures and find that GW0, in general, predicts the band gaps in better agreement with experiments considering the electron-hole effect. For CuCrO2, the HSE wave function is used as the starting point for the perturbative GW0 calculations, since it corrects the band orders wrongly predicted by PBE. The discrepancy about the valence band characters of CuCrO2 is classified based on both HSE and QSGW calculations. The PBE wave functions, already good, are used for other delafossites. All the delafossites are shown to be indirect band gap semiconductors with large exciton binding energies, varying from 0.24 to 0.44 eV, in consistent with experimental findings. The excitation mechanisms are explained by examining the exciton amplitude projections on the band structures. Discrepancies compared with experiments are also addressed. The lowest and strongest exciton, mainly contributed from either Cu 3d → Cu 3p (Al, Ga, In) or Cu 3d → M 3d (M = Sc, Y, Cr) transitions, is always located at the L point of the rhombohedral Brillouin zone.},
doi = {10.1063/1.4991913},
journal = {Journal of Applied Physics},
number = 8,
volume = 122,
place = {United States},
year = {2017},
month = {8}
}

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