Lan Tran Nguyen, Zgid Dominika
Department of Chemistry, University of Michigan , Ann Arbor, Michigan 48109, United States.
Department of Physics, University of Michigan , Ann Arbor, Michigan 48109, United States.
J Phys Chem Lett. 2017 May 18;8(10):2200-2205. doi: 10.1021/acs.jpclett.7b00689. Epub 2017 May 4.
Ab initio quantum chemistry calculations for systems with large active spaces are notoriously difficult and cannot be successfully tackled by standard methods. We generalize a Green's function QM/QM embedding method called self-energy embedding theory (SEET) that has the potential to be successfully employed to treat large active spaces. In generalized SEET, active orbitals are grouped into intersecting groups of a few orbitals, allowing us to perform multiple parallel calculations yielding results comparable to the full active-space treatment. We examine generalized SEET on a series of examples and discuss a hierarchy of systematically improvable approximations.
