Spin-Orbit Interactions in Ultrafast Molecular Processes

Phys Rev Lett. 2020 Jan 24;124(3):033001. doi: 10.1103/PhysRevLett.124.033001.

Abstract

We investigate spin-orbit interactions in ultrafast molecular processes employing the exact factorization of the electron-nuclear wave function. We revisit the original derivation by including spin-orbit coupling, and show how the dynamics driven by the time-dependent potential energy surface alleviates inconsistencies arising from different electronic representations. We propose a novel trajectory-based scheme to simulate spin-forbidden non-radiative processes, and we show its performance in the treatment of excited-state dynamics where spin-orbit effects couple different spin multiplets.