Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 12, Issue 48, Pages 11688-11694Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.1c03229
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- Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences of the U.S. Department of Energy [DE-SC002183]
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The study explores the application of embedding-based methods in electronic excitations of solid-state defects, showing that the DMET method can achieve high accuracy. The practicality of the method is extended and validated in oxygen vacancies on the MgO(100) surface and neutral silicon vacancies in diamond.
Accurate and affordable methods to characterize the electronic structure of solids are important for targeted materials design. Embedding-based methods provide an appealing balance in the trade-off between cost and accuracy-particularly when studying localized phenomena. Here, we use the density matrix embedding theory (DMET) algorithm to study the electronic excitations in solid-state defects with a restricted open-shell Hartree-Fock (ROHF) bath and multireference impurity solvers, specifically, complete active space self-consistent field (CASSCF) and n-electron valence state second-order perturbation theory (NEVPT2). We apply the method to investigate the electronic excitations in an oxygen vacancy (OV) on a MgO(100) surface and find absolute deviations within 0.05 eV between DMET using the CASSCF/NEVPT2 solver, denoted as CAS-DMET/NEVPT2-DMET, and the nonembedded CASSCF/NEVPT2 approach. Next, we establish the practicality of DMET by extending it to larger supercells for the OV defect and a neutral silicon vacancy in diamond where the use of nonembedded CASSCF/NEVPT2 is extremely expensive.
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