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.
Authors
- Tingting Zhao (ORCID: https://orcid.org/0000-0001-8429-2239)
- Devin A. Matthews (ORCID: https://orcid.org/0000-0003-2795-5483)
- James H. Thorpe (ORCID: https://orcid.org/0000-0002-9258-006X)
Institutions
- Southern Methodist University (US)
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
Funders
- National Science Foundation