A self-consistent field formulation of excited state mean field theory [electronic resource]
In this work, we show that, as in Hartree-Fock theory, the orbitals for excited state mean field theory can be optimized via a self-consistent one-electron equation in which electron-electron repulsion is accounted for through mean field operators. In addition to showing that this excited state ansa...
Saved in:
| Online Access: |
Full Text (via OSTI) |
|---|---|
| Corporate Authors: | , |
| Format: | Government Document Electronic eBook |
| Language: | English |
| Published: |
Washington, D.C. : Oak Ridge, Tenn. :
United States. Department of Energy. Office of Science ; Distributed by the Office of Scientific and Technical Information, U.S. Department of Energy,
2020.
|
| Subjects: |
| Summary: | In this work, we show that, as in Hartree-Fock theory, the orbitals for excited state mean field theory can be optimized via a self-consistent one-electron equation in which electron-electron repulsion is accounted for through mean field operators. In addition to showing that this excited state ansatz is sufficiently close to a mean field product state to admit a one-electron formulation, this approach brings the orbital optimization speed to within roughly a factor of two of ground state mean field theory. The approach parallels Hartree Fock theory in multiple ways, including the presence of a commutator condition, a one-electron mean-field working equation, and acceleration via direct inversion in the iterative subspace. When combined with a configuration interaction singles Davidson solver for the excitation coefficients, the self-consistent field formulation dramatically reduces the cost of the theory compared to previous approaches based on quasi-Newton descent. |
|---|---|
| Item Description: | Published through Scitech Connect. 10/28/2020. "Journal ID: ISSN 0021-9606." "Other: ark:/13030/qt223816p1." ": US2204900." Hardikar, Tarini S. ; Neuscamman, Eric ; Lawrence Berkeley National Laboratory, E-Scholarship Repository, Berkeley, CA (United States) |
| Physical Description: | Size: Article No. 164108 : digital, PDF file. |