Broken-Symmetry MO-CI Quantum Master Equation Approach to Exciton Dynamics in Open-Shell Singlet Systems

Recently, we have developed a novel computational approach treating exciton dynamics of supermolecular systems based on the quantum master equation combined with the ab initio molecular orbital - configuration interaction method (MOQME). The MOQME method demonstrates the advantage of describing both coherent and incoherent exciton dynamics in supermolecular systems. In this study, we extend our method to be applicable to the open-shell systems by using broken-symmetry (BS) MO method, referred to as BS-MOQME method. In this formalism, the time evolution of not only the polarization density but also the spin density can be represented based on the MO spatial distributions. A model open-shell system, i.e., H-2 dissociation process, is examined to clarify the applicability of the present scheme.