Quantum embedding theory in the screened Coulomb interaction: Combining configuration interaction with GW/BSE
Dvorak M, Golze D, Rinke P (2019)
Publication Type: Journal article
Publication year: 2019
Journal
Book Volume: 3
Article Number: 070801
Journal Issue: 7
DOI: 10.1103/PhysRevMaterials.3.070801
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(N5) 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 N2, the vertical excitation energies of small molecules, and the ionization spectrum of benzene in excellent agreement with high-level quantum chemistry methods and experiment.
Involved external institutions
Finland (FI)How to cite
APA:
Dvorak, M., Golze, D., & Rinke, P. (2019). Quantum embedding theory in the screened Coulomb interaction: Combining configuration interaction with GW/BSE. Physical Review Materials, 3(7). https://doi.org/10.1103/PhysRevMaterials.3.070801
MLA:
Dvorak, Marc, Dorothea Golze, and Patrick Rinke. "Quantum embedding theory in the screened Coulomb interaction: Combining configuration interaction with GW/BSE." Physical Review Materials 3.7 (2019).
BibTeX: Download