Abstract
Molecular and lattice vibrations are able to couple to the spin of electrons and lead to their relaxation and decoherence. Ab initio simulations have played a fundamental role in shaping our understanding of this process but further progress is hindered by their high computational cost. Here we present an accelerated computational framework based on machine-learning models for the prediction of molecular vibrations and spin-phonon coupling coefficients. We apply this method to three open-shell coordination compounds exhibiting long relaxation times and show that this approach achieves semi-to-full quantitative agreement with ab initio methods reducing the computational cost by about 80%. Moreover, we show that this framework naturally extends to molecular dynamics simulations, paving the way to the study of spin relaxation in condensed matter beyond simple equilibrium harmonic thermal baths.