Real-Time CASSCF (Ehrenfest) Modeling of Electron Dynamics in Organic Semiconductors. Dynamics Reaction Paths Driven by Quantum Coherences. Application to a Radical Organic Semiconductor.

We present a strategy for the modeling of charge carrier dynamics in organic semiconductors using conventional quantum chemistry methods, including the analytic gradient for nuclear motion. The theoretical approach uses real-time CASSCF (Ehrenfest) all-electron dynamics coupled to classical nuclear dynamics for the special case of a small number (4-8) of molecular units. The objective is to obtain mechanistic/atomistic insight at the electronic structure level, relating to spin density dynamics, to the effect of crystal structure (e.