Near-Linear Scaling in DMRG-Based Tailored Coupled Clusters: An Implementation of DLPNO-TCCSD and DLPNO-TCCSD(T)

0524283 - ÚFCH JH 2021 RIV US eng J - Článek v odborném periodiku
Lang, Jakub - Antalík, Andrej - Veis, Libor - Brandejs, Jan - Brabec, Jiří - Legeza, Ö. - Pittner, Jiří
Near-Linear Scaling in DMRG-Based Tailored Coupled Clusters: An Implementation of DLPNO-TCCSD and DLPNO-TCCSD(T).
Journal of Chemical Theory and Computation. Roč. 16, č. 5 (2020), s. 3028-3040. ISSN 1549-9618. E-ISSN 1549-9626
Grant CEP: GA ČR(CZ) GA18-24563S; GA ČR GA16-12052S; GA ČR(CZ) GJ18-18940Y; GA MŠMT(CZ) LTAUSA17033
Grant ostatní: Ga MŠk(CZ) LM2015070; AV ČR(CZ) MTA-19-04
Program: Bilaterální spolupráce
Institucionální podpora: RVO:61388955
Klíčová slova: Energy * Basis sets * Quantum mechanics * Chemical calculations
Obor OECD: Physical chemistry
Impakt faktor: 6.006, rok: 2020
Způsob publikování: Omezený přístup

We present a new implementation of density matrix renormalization group based tailored coupled clusters method (TCCSD), which employs the domain-based local pair natural orbital approach (DLPNO). Compared to the previous local pair natural orbital (LPNO) version of the method, the new implementation is more accurate, offers more favorable scaling, and provides more consistent behavior across the variety of systems. On top of the singles and doubles, we include the perturbative triples correction (T), which is able to retrieve even more dynamic correlation. The methods were tested on three systems: tetramethyleneethane, oxo-Mn(Salen), and iron(II)–porphyrin model. The first two were revisited to assess the performance with respect to LPNO-TCCSD. For oxo-Mn(Salen), we retrieved between 99.8 and 99.9% of the total canonical correlation energy which is an improvement of 0.2% over the LPNO version in less than 63% of the total LPNO runtime. Similar results were obtained for iron(II)–porphyrin. When the perturbative triples correction was employed, irrespective of the active space size or system, the obtained energy differences between two spin states were within the chemical accuracy of 1 kcal/mol using the default DLPNO settings.
Trvalý link: http://hdl.handle.net/11104/0308654