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Efficient Formulation of Ab Initio Quantum Embedding in Periodic Systems: Dynamical Mean-Field Theory

Zhu, Tianyu and Cui, Zhi-Hao and Chan, Garnet Kin-Lic (2020) Efficient Formulation of Ab Initio Quantum Embedding in Periodic Systems: Dynamical Mean-Field Theory. Journal of Chemical Theory and Computation, 16 (1). pp. 141-153. ISSN 1549-9618. doi:10.1021/acs.jctc.9b00934.

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We present an efficient ab initio dynamical mean-field theory (DMFT) implementation for quantitative simulations in solids. Our DMFT scheme employs ab initio Hamiltonians defined for impurities comprising the full unit cell or a supercell of atoms and for realistic quantum chemical basis sets. We avoid double counting errors by using Hartree–Fock as the low-level theory. Intrinsic and projected atomic orbitals (IAO + PAO) are chosen as the local embedding basis, facilitating numerical bath truncation. Using an efficient integral transformation and coupled-cluster Green’s function impurity solvers, we are able to handle embedded impurity problems with several hundred orbitals. We apply our ab initio DMFT approach to study a hexagonal boron nitride monolayer, crystalline silicon, and nickel oxide in the antiferromagnetic phase, with up to 104 and 78 impurity orbitals in the spin-restricted and unrestricted cluster DMFT calculations and over 100 bath orbitals. We show that our scheme produces accurate spectral functions compared to both benchmark periodic coupled-cluster computations and experimental spectra.

Item Type:Article
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URLURL TypeDescription Paper
Zhu, Tianyu0000-0003-2061-3237
Cui, Zhi-Hao0000-0002-7389-4063
Chan, Garnet Kin-Lic0000-0001-8009-6038
Additional Information:© 2019 American Chemical Society. Received: September 19, 2019; Published: December 9, 2019. We thank Timothy Berkelbach and Yang Gao for helpful discussions. This work is supported by the US DOE via DE-SC0018140. 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.
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Department of Energy (DOE)DE-SC0018140
Simons FoundationUNSPECIFIED
Issue or Number:1
Record Number:CaltechAUTHORS:20191210-142224886
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Official Citation:Efficient Formulation of Ab Initio Quantum Embedding in Periodic Systems: Dynamical Mean-Field Theory. Tianyu Zhu, Zhi-Hao Cui, and Garnet Kin-Lic Chan. Journal of Chemical Theory and Computation 2020 16 (1), 141-153; DOI: 10.1021/acs.jctc.9b00934
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:100267
Deposited By: Tony Diaz
Deposited On:10 Dec 2019 22:27
Last Modified:16 Nov 2021 17:52

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