An attractive way to correct for missing singles excitations in unitary coupled cluster doubles theory

• URL: http://arxiv.org/abs/2406.09174v1
• Date: Thu, 13 Jun 2024 14:36:15 GMT
• Title: An attractive way to correct for missing singles excitations in unitary coupled cluster doubles theory
• Authors: Zachary W. Windom, Daniel Claudino, Rodney J. Bartlett,
• Abstract summary: We investigate the extent in which missing single excitations can be recovered from low-order perturbations in many-body theory. Our analysis includes the derivations of finite-order, UCC energy functionals. We show that augmenting UCCD with these post hoc perturbative corrections can lead to UCCSD-quality results.
• Score: 0.0
• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: Coupled cluster methods based exclusively on double excitations are comparatively "cheap" and interesting model chemistries, as they are typically able to capture the bulk of the dynamical electron correlation effects. The trade-off in such approximations is that the effect of neglected excitations, particularly single excitations, can be considerable. Using standard and electron pair-restricted $T_2$ operators to define two flavors of unitary coupled cluster doubles (UCCD) methods, we investigate the extent in which missing single excitations can be recovered from low-order corrections in many-body perturbation theory (MBPT) within the unitary coupled cluster (UCC) formalism. Our analysis includes the derivations of finite-order, UCC energy functionals which are used as a basis to define perturbative estimates of missed single excitations. This leads to the novel UCCD[4S] and UCCD[6S] methods, which consider energy corrections for missing singles excitations through fourth- and sixth-order in MBPT, respectively. We also apply the same methodology to the electron pair-restricted ansatz, but the improvements are only marginal. Our findings show that augmenting UCCD with these post hoc perturbative corrections can lead to UCCSD-quality results.

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