Embedding methods for Electronic Structure can provide accurate descriptions of chemical reactions
Welborn, M., Manby, F., Miller, T. Even-handed subsystem selection in projection-based embedding. The Journal of Chemical Physics, 149, 144101, DOI: https://doi.org/10.1063/1.5050533 (2018)
By treating different parts of a chemical system with different levels of theory, embedding methods for electronic structure can provide accurate description of chemical reactions at reduced computational cost.
In this paper, researchers looked at projection-based embedding that offers a simple framework for embedding correlated wavefunction methods in density functional theory. During a large geometry change—such as a chemical reaction—the nature of these localized molecular orbitals, as well as their partitioning into the two subsystems, can change dramatically. This work presents an even-handed framework for localized orbital partitioning that ensures consistent subsystems across a set of molecular geometries. SN2 reactions were used as illustrations of this approach. Applications to a nitrogen umbrella flip in a cobalt-based CO2 reduction catalyst and to the binding of CO to Cu clusters are presented in the paper.