Tensor Hypercontraction of Cluster Perturbation Theory: Quartic Scaling Perturbation Series for the Coupled Cluster Singles and Doubles Ground-State Energies

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Even though cluster perturbation theory has been shown to be a robust noniterative alternative to coupled cluster theory, it is still plagued by high order polynomial computational scaling and the storage of higher order tensors. We present a proof-of-concept strategy for implementing a cluster perturbation theory ground-state energy series for the coupled cluster singles and doubles energy with N4 computational scaling using tensor hypercontraction (THC). The reduction in computational scaling by two orders is achieved by decomposing two electron repulsion integrals, doubles amplitudes and multipliers, as well as selected double intermediates to the THC format. Using the outlined strategy, we showcase that the THC pilot implementations retain numerical accuracy to within 1 kcal/mol relative to corresponding conventional and density fitting implementations, and we empirically verify the N4 scaling.

Original languageEnglish
JournalJournal of Chemical Theory and Computation
Volume20
Issue number5
Pages (from-to)1932-1943
Number of pages12
ISSN1549-9618
DOIs
Publication statusPublished - 2024

Bibliographical note

Funding Information:
A.E.H.-B. acknowledges generous financial support from the Ministry of Higher Education and Research, Denmark, which funded a stay with T.J.M. at Stanford University and SLAC National Accelerator Laboratory during which this research was conducted. T.J.M. acknowledges support from the AMOS program of the Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences and Biosciences Division. A.E.H.-B. and K.V.M. acknowledge financial support from the European Commission (grant no. 765739) and the Danish Council for Independent Research, DFF-0136-00081B.

Publisher Copyright:
© 2024 American Chemical Society.

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