In this work, 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.
Zhu, Tianyu, et al. "Efficient Formulation of Ab Initio Quantum Embedding in Periodic Systems: Dynamical Mean-Field Theory." Journal of Chemical Theory and Computation, vol. 16, no. 1, Dec. 2019. https://doi.org/10.1021/acs.jctc.9b00934
Zhu, Tianyu, Cui, Zhi-Hao, & Chan, Garnet Kin-Lic (2019). Efficient Formulation of Ab Initio Quantum Embedding in Periodic Systems: Dynamical Mean-Field Theory. Journal of Chemical Theory and Computation, 16(1). https://doi.org/10.1021/acs.jctc.9b00934
Zhu, Tianyu, Cui, Zhi-Hao, and Chan, Garnet Kin-Lic, "Efficient Formulation of Ab Initio Quantum Embedding in Periodic Systems: Dynamical Mean-Field Theory," Journal of Chemical Theory and Computation 16, no. 1 (2019), https://doi.org/10.1021/acs.jctc.9b00934
@article{osti_1803262,
author = {Zhu, Tianyu and Cui, Zhi-Hao and Chan, Garnet Kin-Lic},
title = {Efficient Formulation of Ab Initio Quantum Embedding in Periodic Systems: Dynamical Mean-Field Theory},
annote = {In this work, 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.},
doi = {10.1021/acs.jctc.9b00934},
url = {https://www.osti.gov/biblio/1803262},
journal = {Journal of Chemical Theory and Computation},
issn = {ISSN 1549-9618},
number = {1},
volume = {16},
place = {United States},
publisher = {American Chemical Society},
year = {2019},
month = {12}}