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Addressing the System-Size Dependence of the Local Approximation Error in Coupled-Cluster Calculations.

ABSTRACT: Over the last two decades, the local approximation has been successfully used to extend the range of applicability of the "gold standard" singles and doubles coupled-cluster method with perturbative triples CCSD(T) to systems with hundreds of atoms. The local approximation error grows in absolute value with the increasing system size, i.e., by increasing the number of electron pairs in the system. In this study, we demonstrate that the recently introduced two-point extrapolation scheme for approaching the complete pair natural orbital (PNOs) space limit in domain-based pair natural orbital CCSD(T) calculations drastically reduces the dependence of the error on the system size, thus opening up unprecedented opportunities for the calculation of benchmark quality relative energies for large systems.

SUBMITTER: Altun A

PROVIDER: S-EPMC8607505 | biostudies-literature | 2021 Nov

REPOSITORIES: biostudies-literature

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Addressing the System-Size Dependence of the Local Approximation Error in Coupled-Cluster Calculations.

Altun Ahmet A Ghosh Soumen S Riplinger Christoph C Neese Frank F Bistoni Giovanni G

The journal of physical chemistry. A 20211103 45

Over the last two decades, the local approximation has been successfully used to extend the range of applicability of the "gold standard" singles and doubles coupled-cluster method with perturbative triples CCSD(T) to systems with hundreds of atoms. The local approximation error grows in absolute value with the increasing system size, i.e., by increasing the number of electron pairs in the system. In this study, we demonstrate that the recently introduced two-point extrapolation scheme for appro ...[more]

PMID: 34730360

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