Journal
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
Volume 16, Issue 1, Pages 141-153Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jctc.9b00934
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Funding
- US DOE [DE-SC0018140]
- Simons Foundation via the Simons Collaboration on the ManyElectron Problem
- Simons Foundation via the Simons Investigatorship in Physics
- U.S. Department of Energy (DOE) [DE-SC0018140] Funding Source: U.S. Department of Energy (DOE)
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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.
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