Flexible Framework for Surface Hopping: From Hybrid Schemes for Machine Learning to Benchmarkable Nonadiabatic Dynamics

TL;DR

This paper introduces a flexible, open-source framework in MLatom for nonadiabatic molecular dynamics using surface hopping, facilitating machine learning integration, benchmarking, and detailed trajectory analysis.

Contribution

It presents a new implementation of surface hopping algorithms within MLatom, enabling customizable models, benchmarking, and analysis tools for nonadiabatic dynamics.

Findings

Landau--Zener scheme outperforms Baeck--An in curvature-driven surface hopping.

Custom models reduce computational time and aid benchmarking.

Framework supports detailed analysis of trajectories and ensembles.

Abstract

Nonadiabatic molecular dynamics is a key technique for investigating a broad range of photochemical and photophysical processes. Among the established approaches, surface hopping schemes are widely used and can be easily integrated with various quantum chemistry programs or machine learning models. We present a flexible framework in MLatom that includes a newly implemented Tully's fewest-switches surface hopping algorithm and its time-dependent Baeck--An variant. The capabilities of this framework are demonstrated through three representative examples corresponding to typical stages of a surface hopping study. First, we focus on methods providing energy, energy gradients and nonadiabatic couplings. We show that the flexibility of user-defined custom models can save computational time and that it is useful for benchmarking machine learning models. Next, we compare curvature-driven surface hopping schemes and show that Landau--Zener approach outperforms the time-dependent Baeck--An scheme. Finally, we showcase easy-to-use analysis tools for both individual trajectories and trajectory ensembles. This framework enables accelerated development of machine learning models and provides deeper insight into nonadiabatic dynamics. It is available as a part of the open-source MLatom package.