Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 146, Issue 9, Pages -Publisher
AMER INST PHYSICS
DOI: 10.1063/1.4976644
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Funding
- JSPS Kakenhi [JP15K20832, JP15H03770]
- JST-CREST
- Building of Consortia for the Development of Human Resources in Science and Technology, MEXT, Japan
- NSF [NSF-CHE 1657286]
- Grants-in-Aid for Scientific Research [15K20832] Funding Source: KAKEN
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This paper describes an interface between the density matrix renormalization group (DMRG) method and the complete active-space self-consistent field (CASSCF) method and its analytical gradient, as well as an extension to the second-order perturbation theory (CASPT2) method. This interfacing allows large active-space multi-reference computations to be easily performed. The interface and its extension are both implemented in terms of reduced density matrices (RDMs) which can be efficiently computed via the DMRG sweep algorithm. We also present benchmark results showing that, in practice, the DMRG-CASSCF calculations scale with active-space size in a polynomial manner in the case of quasi-1D systems. Geometry optimization of a binuclear iron-sulfur cluster using the DMRG-CASSCF analytical gradient is demonstrated, indicating that the inclusion of the valence p-orbitals of sulfur and double-shell d-orbitals of iron lead to non-negligible changes in the geometry compared to the results of small active-space calculations. With the exception of the selection of M values, many computational settings in these practical DMRG calculations have been tuned and black-boxed in our interface, and so the resulting DMRG-CASSCF and DMRG-CASPT2 calculations are now available to novice users as a common tool to compute strongly correlated electronic wavefunctions. Published by AIP Publishing.
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