Transferable machine learning of excited-state dynamics with extremal pooling

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Original abstract

Photochemical processes govern phenomena ranging from solar energy conversion and atmospheric chemistry to vision and photosynthesis. Accurate simulation of these processes requires modeling excited-state potential energy surfaces, often involving chemical reactions, tasks that remain computationally prohibitive for extended systems and long timescales using traditional \textit{ab initio} methods. Machine learning interatomic potentials have revolutionized ground-state simulations, but their extension to excited states faces fundamental challenges: standard architectures assume energy extensivity, an assumption that fails for excited states. Here, we present a size-intensive machine-learning framework for excited-state dynamics based on \textit{extremal pooling} of predicted atomic HOMO and LUMO contributions. Trained exclusively on excitations energies and forces, the architecture learns interpretable atomic-level contributions that encode physical information on the extent of electron localization. We demonstrate this framework on the photoexcited solvated electron in liquid water, a paradigmatic problem in radiation chemistry leading to competing pathways involving both hydrogen-atom dissociation and proton-coupled electron transfer. The model not only reproduces the relevant chain of reactions and product species that form during excitation, but also allows one to explicitly study the dynamics of the solvated electron in quantitative agreement with previously reported Restricted Open-Shell Kohn-Sham calculations, while enabling excited-state simulations of periodic systems at length and time scales inaccessible to the reference electronic-structure method. This work establishes a general strategy for machine learning-driven excited-state dynamics applicable to diverse photochemical systems, from molecular chromophores in solution to extended condensed-phase systems.

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