Time propagation of electronic wavefunctions using nonorthogonal determinant expansions

Dong, Xinju; Thompson, Lee M.

doi:10.1063/5.0179601

Title: Time propagation of electronic wavefunctions using nonorthogonal determinant expansions

Journal Article · 07 January 2024 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/5.0179601 · OSTI ID:2281688

^[1];

^[2]

Univ. of Louisville, KY (United States); University of Louisville
Univ. of Louisville, KY (United States)

The use of truncated configuration interaction in real-time time-dependent simulations of electron dynamics provides a balance of computational cost and accuracy, while avoiding some of the failures associated with real-time time-dependent density functional theory. However, low-order truncated configuration interaction also has limitations, such as overestimation of polarizability in configuration interaction singles, even when perturbative doubles are included. Increasing the size of the determinant expansion may not be computationally feasible, and so, in this work, we investigate the use of nonorthogonality in the determinant expansion to establish the extent to which higher-order substitutions can be recovered, providing an improved description of electron dynamics. Model systems are investigated to quantify the extent to which different methods accurately reproduce the (hyper)polarizability, including the high-harmonic generation spectrum of H₂, water, and butadiene.

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Research Organization:: Univ. of Louisville, KY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0024507

OSTI ID:: 2281688

Report Number(s):: DOE-LOUISVILLE--24507

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 2 Vol. 160; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Time propagation of electronic wavefunctions using nonorthogonal determinant expansions

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