Spin Currents Induced in Open-Shell Molecules by Static and Uniform Magnetic and Electric Fields in the Presence of a Spin-Orbit Coupling Interaction and Conservation Law

J Chem Theory Comput. 2023 May 9;19(9):2491-2501. doi: 10.1021/acs.jctc.3c00017. Epub 2023 Apr 27.

Abstract

The derivation of the total induced current density vector field, in the presence of static and uniform magnetic and electric fields, is illustrated in a more clear and formally correct language together with a discussion on the charge-current conservation law not presented before for the spin-orbit coupling contribution. The theory here exposed turns out to be in fully agreement with the theory of Special Relativity and it is applicable to open-shell molecules in the presence of a nonvanishing spin orbit coupling. The discussion here exposed turns out to be accurately valid for a strictly central field due to the chosen approximation of the spin-orbit coupling Hamiltonian, but it is appropriate to deal correctly with molecular systems. The ab initio calculation of spin current densities has been implemented at both unrestricted Hartree-Fock and unrestricted DFT levels of theory. Some maps of spin currents on molecules of interest, i.e., the CH3 radical and the superoctazethrene molecule are also illustrated.