Quantum embedding theory in the screened Coulomb interaction: Combining configuration interaction with GW/BSE
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A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
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Date
2019-07-31
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Language
en
Pages
6
1-6
1-6
Series
Physical Review Materials, Volume 3, issue 7
Abstract
We present a quantum embedding theory called dynamical configuration interaction (DCI) that combines wave function and Green's function theories. DCI captures static correlation in a correlated subspace with configuration interaction and couples to high-energy, dynamic correlation outside the subspace with many-body perturbation theory based on Green's functions. DCI takes the strengths of both theories to balance static and dynamic correlation in a single, fully ab initio embedding concept. The theory adds dynamic correlation around a fixed active space of orbitals with efficient O(N-5) scaling, while maintaining a multireference treatment of the active space. We show that treating high-energy correlation up to the GW and Bethe-Salpeter equation level is sufficient even for challenging multireference problems. Our theory treats ground and excited states on equal footing, and we compute the dissociation curve of N-2, the vertical excitation energies of small molecules, and the ionization spectrum of benzene in excellent agreement with high-level quantum chemistry methods and experiment.Description
Keywords
PERTURBATION-THEORY, EXCITED-STATES, ELECTRON, BUTADIENE, ETHYLENE, VALENCE, SPECTROSCOPY, BENCHMARKING, EXCITATIONS, EQUATION
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Citation
Dvorak, M, Golze, D & Rinke, P 2019, ' Quantum embedding theory in the screened Coulomb interaction : Combining configuration interaction with GW/BSE ', Physical Review Materials, vol. 3, no. 7, 070801, pp. 1-6 . https://doi.org/10.1103/PhysRevMaterials.3.070801
