Matthew R Hermes, Bhavnesh Jangid, Valay Agarawal, Laura Gagliardi
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Abstract
We introduce localized active space state interaction singles (LASSIS), a multireference electronic structure method that uses two-step diagonalization to model low-energy electronic states of systems characterized by multiple distinct localized centers of strong electron correlation, with weaker but not negligible electron correlation between the centers. LASSIS is a specific variant of localized active space state interaction (LASSI), which restores interfragment interactions omitted by a LASSCF reference wave function by expanding the interacting wave function in a basis of model states characterized by various charge and spin distributions. These distributions, and the number of states of each type, are determined automatically, without any user input, in contrast to previous work with the LASSI formalism. LASSIS combined with multiconfiguration pair-density functional theory (MC-PDFT) energy calculation is shown in test calculations to qualitatively reproduce the results of converged DMRG-PDFT calculations on multimetallic transition metal compounds.
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The Journal of Chemical Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere. Papers reporting new theories, methodology, and/or important applications in quantum electronic structure, molecular dynamics, and statistical mechanics are appropriate for submission to this Journal. Specific topics include advances in or applications of ab initio quantum mechanics, density functional theory, design and properties of new materials, surface science, Monte Carlo simulations, solvation models, QM/MM calculations, biomolecular structure prediction, and molecular dynamics in the broadest sense including gas-phase dynamics, ab initio dynamics, biomolecular dynamics, and protein folding. The Journal does not consider papers that are straightforward applications of known methods including DFT and molecular dynamics. The Journal favors submissions that include advances in theory or methodology with applications to compelling problems.
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