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 proce...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 semito-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.展开更多
基金funding from the European Research Council(ERC)under the European Union’s Horizon 2020 research and innovation programme(grant agreement No.[948493])Computational resources were provided by the Trinity College Research IT and the Irish Centre for High-End Computing(ICHEC).
文摘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 semito-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.
