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Generalized single excitation configuration interaction: an investigation into the impact of the inclusion of non-orthogonality on the calculation of core-excited states

Journal Article · · Physical Chemistry Chemical Physics. PCCP
DOI:https://doi.org/10.1039/c9cp06592j· OSTI ID:1779241
 [1];  [2];  [1];  [1]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Div.
  2. California Institute of Technology (CalTech), Pasadena, CA (United States). Div. of Chemistry and Chemical Engineering
In this paper, we investigate different non-orthogonal generalizations of the configuration interaction with single substitutions (CIS) method for the calculation of core-excited states. Fully non-orthogonal CIS (NOCIS) has been described previously for species with singlet and doublet ground states, and this paper reports the extension to molecules in their triplet ground state. In addition to NOCIS, we present a novel method, one-center NOCIS (1C-NOCIS), for open-shell molecules which is intermediate between NOCIS and the computationally less demanding static exchange approximation (STEX). We explore this hierarchy of spin-pure methods for core excitations of molecules with singlet, doublet, and triplet ground states. We conclude that, while NOCIS provides the best results and preserves the spatial symmetry of the wavefunction, 1C-NOCIS retains much of the accuracy of NOCIS at a dramatically reduced cost. For molecules with closed-shell ground states, STEX and 1C-NOCIS are identical.
Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1779241
Alternate ID(s):
OSTI ID: 1608381
Journal Information:
Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 15 Vol. 22; ISSN 1463-9076
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

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