Machine-learning-accelerated photodynamics simulations in complex environments towards new materials and medicines

Steven A. Lopez

Photochemical reactions are increasingly important for constructing value-added, strained organic architectures. Direct excitation and photoredox reactions typically require mild conditions to access therapeutic gases (e.g., carbon monoxide) and new synthetic methodologies. A priori design of photochemical reactions is challenging because degenerate excited states often result in competing reaction mechanisms to undesired products. Further, a lack of experimental techniques that provide atomistic structural information on ultrafast timescales (10–15 – 10–12 s) has limited general rules about these reactions. Computations, however, provide a path forward. I will discuss how my group has leveraged multiconfigurational complete active space self consistent field (CASSCF) calculations, non-adiabatic molecular dynamics, and machine learning (ML) techniques to understand reaction mechanisms and enumerate new reaction pathways. I will introduce our new open-access machine learning tool, Python Rapid Artificial Intelligence Ab Initio Molecular Dynamics (PyRAI2MD), which enables 100,000-fold longer simulations than current NAMD simulations with multiconfigurational quantum chemical methods. I will describe how PyRAI2MD has enabled the first ML-NAMD simulations with QM (CAS/HF) training data. The presentation will explain the origins of the reactivities and selectivities of photochemical pericyclic reactions and CO-evolving reactions in aqueous environments.