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All-Electron Gaussian-Based G₀W₀ for Valence and Core Excitation Energies of Periodic Systems

Zhu, Tianyu and Chan, Garnet Kin-Lic (2021) All-Electron Gaussian-Based G₀W₀ for Valence and Core Excitation Energies of Periodic Systems. Journal of Chemical Theory and Computation, 17 (2). pp. 727-741. ISSN 1549-9618. doi:10.1021/acs.jctc.0c00704.

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We describe an all-electron G₀W₀ implementation for periodic systems with k-point sampling implemented in a crystalline Gaussian basis. Our full-frequency G₀W₀ method relies on efficient Gaussian density fitting integrals and includes both analytic continuation and contour deformation schemes. Due to the compactness of Gaussian bases, no virtual state truncation is required as is seen in many plane-wave formulations. Finite size corrections are included by taking the q → 0 limit of the Coulomb divergence. Using our implementation, we study quasiparticle energies and band structures across a range of systems including molecules, semiconductors, rare gas solids, and metals. We find that the G₀W₀ band gaps of traditional semiconductors converge rapidly with respect to the basis size, even for the conventionally challenging case of ZnO. Using correlation-consistent bases of polarized triple-ζ quality, we find the mean absolute relative error of the extrapolated G₀W₀@PBE band gaps to be only 5.2% when compared to experimental values. For core excitation binding energies (CEBEs), we find that G₀W₀ predictions improve significantly over those from DFT if the G₀W₀ calculations are started from hybrid functionals with a high percentage of exact exchange.

Item Type:Article
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URLURL TypeDescription Paper
Zhu, Tianyu0000-0003-2061-3237
Chan, Garnet Kin-Lic0000-0001-8009-6038
Alternate Title:All-Electron Gaussian-Based G0W0 for Valence and Core Excitation Energies of Periodic Systems
Additional Information:© 2020 American Chemical Society. Received: July 7, 2020; Published: January 5, 2021. This work was supported by the U.S. Department of Energy, Office of Science under award no. 19390. T.Z. thanks Zhihao Cui, Yang Gao, and Timothy Berkelbach for helpful discussions. Additional support was provided by the Simons Foundation via the Simons Collaboration on the Many Electron Problem and via the Simons Investigatorship in Physics. The authors declare no competing financial interest.
Funding AgencyGrant Number
Department of Energy (DOE)19390
Simons FoundationUNSPECIFIED
Issue or Number:2
Record Number:CaltechAUTHORS:20200811-091206924
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Official Citation:All-Electron Gaussian-Based G0W0 for Valence and Core Excitation Energies of Periodic Systems. Tianyu Zhu and Garnet Kin-Lic Chan. Journal of Chemical Theory and Computation 2021 17 (2), 727-741; DOI: 10.1021/acs.jctc.0c00704
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:104904
Deposited By: Tony Diaz
Deposited On:11 Aug 2020 16:42
Last Modified:16 Nov 2021 18:37

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