Learning Decoherence Time Formulas for Surface Hopping from Quantum Dynamics.

Surface hopping simulations have achieved great success in many different fields, but their reliability has long been limited by the overcoherence problem. We here present a general machine learning assisted approach to identify optimal decoherence time formulas for surface hopping using exact quantum dynamics as references. In order to avoid computationally expensive force calculations, we use the nuclear kinetic energy and the adiabatic energy difference to iteratively generate the descriptor space. Through multilayer screening of the candidate descriptors and discrete optimization of the relevant parameters, we obtain new energy-based decoherence time formulas. As benchmarked in thousands of diverse multilevel systems and six standard scattering models, surface hopping with our new decoherence time formulas nearly reproduces the exact quantum dynamics while maintaining high efficiency. Thereby, our approach provides a promising avenue for systematically improving the accuracy of surface hopping simulations in complex systems from quantum dynamics data.