Spin-Dependent Stereochemistry: A Non-adiabatic Quantum Dynamics Case Study of S + H2 -> SH + H Reaction

Abstract

We study the spin-dependent stereodynamics of the S + H2 -> SH + H reaction using full-dimensional quantum dynamics calculations with zero total nuclear angular momentum along the triplet 3A" states and singlet 1A' states. We find that the interplay between the electronic spin direction and the molecular geometry has a measurable influence on the singlet-triplet intersystem crossing reaction probabilities. Our results show that for some incident scattering angles in the body-fixed frame, the relative difference in intersystem crossing reaction probabilities (as determined between spin up and spin down initial states) can be as large as 15%. Our findings are an ab initio demonstration of spin-dependent nonadiabatic dynamics which we hope will shine light as far as understanding the chiral-induced spin selectivity effect.