Kantorovich dual solution for strictly correlated electrons in atoms and molecules

The many-body Coulomb repulsive energy of strictly correlated electrons provides direct information on the exact Hohenberg-Kohn exchange-correlation functional in the strong interaction limit. Until now the treatment of strictly correlated electrons has been based on the calculation of comotion functions with the help of semianalytic formulations. This procedure is system-specific and has been limited to spherically symmetric atoms and strictly one-dimensional systems. We develop a nested optimization method which solves the Kantorovich dual problem directly, and thus facilitates a general treatment of strictly correlated electrons for systems including atoms and small molecules. DOI: 10.1103/PhysRevB.87.125106