Prospects for rank-reduced CCSD(T) in the context of high-accuracy thermochemistry

Obtaining sub-chemical accuracy (1 kJ mol-1) for reaction energies of medium-sized gas-phase molecules is a longstanding challenge in the field of thermochemical modeling. The perturbative triples correction to coupled-cluster single double triple [CCSD(T)] constitutes an important component of all high-accuracy composite model chemistries that obtain this accuracy but can be a roadblock in the calculation of medium to large systems due to its O(N7) scaling, particularly in HEAT-like model chemistries that eschew separation of core and valence correlation. This study extends the work of Lesiuk [J. Chem. Phys. 156, 064103 (2022)] with new approximate methods and assesses the accuracy of five different approximations of (T) in the context of a subset of molecules selected from the W4-17 dataset. It is demonstrated that all of these approximate methods can achieve sub-0.1 kJ mol-1 accuracy with respect to canonical, density-fitted (T) contributions with a modest number of projectors. The approximation labeled Z̃T appears to offer the best trade-off between cost and accuracy and shows significant promise in an order-of-magnitude reduction in the computational cost of the CCSD(T) component of high-accuracy model chemistries.

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Publication Details

Journal
The Journal of Chemical Physics
Published
2024-10-18
DOI
https://doi.org/10.1063/5.0230899
Citations
2
Primary Topic
Advanced Chemical Physics Studies
Type
article
Field-Weighted Citation Impact
0.68

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article

Prospects for rank-reduced CCSD(T) in the context of high-accuracy thermochemistry

Tingting Zhao, Devin A. Matthews, James H. Thorpe
2 citations
The Journal of Chemical Physics
Advanced Chemical Physics Studies
0.68
article

Prospects for rank-reduced CCSD(T) in the context of high-accuracy thermochemistry

Tingting Zhao, Devin A. Matthews, James H. Thorpe
article en
2 citations

Abstract

Obtaining sub-chemical accuracy (1 kJ mol-1) for reaction energies of medium-sized gas-phase molecules is a longstanding challenge in the field of thermochemical modeling. The perturbative triples correction to coupled-cluster single double triple [CCSD(T)] constitutes an important component of all high-accuracy composite model chemistries that obtain this accuracy but can be a roadblock in the calculation of medium to large systems due to its O(N7) scaling, particularly in HEAT-like model chemistries that eschew separation of core and valence correlation. This study extends the work of Lesiuk [J. Chem. Phys. 156, 064103 (2022)] with new approximate methods and assesses the accuracy of five different approximations of (T) in the context of a subset of molecules selected from the W4-17 dataset. It is demonstrated that all of these approximate methods can achieve sub-0.1 kJ mol-1 accuracy with respect to canonical, density-fitted (T) contributions with a modest number of projectors. The approximation labeled Z̃T appears to offer the best trade-off between cost and accuracy and shows significant promise in an order-of-magnitude reduction in the computational cost of the CCSD(T) component of high-accuracy model chemistries.

The Journal of Chemical PhysicsVol. 161(15)
Southern Methodist University (US)
National Science Foundation
Openalex Percentile: Top 30%
Advanced Chemical Physics Studies
0.68
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