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Relativistic Two-Component Multireference Configuration Interaction Method with Tunable Correlation Space

Cite this: J. Chem. Theory Comput. 2020, 16, 5, 2975–2984
Publication Date (Web):April 10, 2020
https://doi.org/10.1021/acs.jctc.9b01290
Copyright © 2020 American Chemical Society

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    Abstract

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    The multiconfiguration nature of late-row (≥4th) elements and their molecular complexes, combined with significant relativistic effects, present large challenges for the accurate description of their electronic structure. To address these challenges and incorporate both relativistic and electron correlation effects, we present a two-component Kramers-unrestricted multireference configuration interaction method where relativistic effects are included variationally at the molecular orbital level via use of the “exact two-component” transformation of the solution of the one-electron modified Dirac equation. This method is developed within the restricted active space framework, allowing flexibility in both the choice of correlation space and the level of truncation of the excitation operator, as well as promoting the efficiency of generating and book-keeping unique electronic configurations. This method is applied to the study of fine structure splitting in selected p-block and d-block elements and is further applied to the study of the open-shell heavy-element uranium(V) ion.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jctc.9b01290.

    • Basis set and comparison of 4C-CASSCF and X2C-SA-CASSCF; convergence of the X2C-MRCI virtual space; and effects of core electrons (PDF)

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    This article is cited by 30 publications.

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