2024/01/15 by Sebastian V. Pios, Maxim F. Gelin, Pios, Sebastian V. +7
Chemistry · Neuroscience · Physics and Astronomy · #Chemical Physics (physics.chem-ph) #FOS: Physical sciences #Photochemistry and Electron Transfer Studies #Photoreceptor and optogenetics research #Spectroscopy and Quantum Chemical Studies
paper · pdf · doi:10.48550/arxiv.2401.07399
openalex publication_date 2024/01/15 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28
Time-resolved spectroscopy is an important tool for unraveling the minute details of structural changes of molecules of biological and technological significance. The nonlinear femtosecond signals detected for such systems must be interpreted, but it is a challenging task for which theoretical simulations are often indispensable. Accurate simulations of transient-absorption or two-dimensional electronic spectra are, however, computationally very expensive, prohibiting the wider adoption of existing first-principles methods. Here, we report an AI-enhanced protocol to drastically reduce the computational cost of simulating nonlinear time-resolved electronic spectra which makes such simulations affordable for polyatomic molecules of increasing size. The protocol is based on doorway-window approach for the on-the-fly surface-hopping simulations. We show its applicability for the prototypical molecule of pyrazine for which it produces spectra with high precision with respect to ab initio reference while cutting the computational cost by at least 95% compared to pure first-principles simulations.