Deciphering the Influence of Ground-State Distributions on the Calculation of Photolysis Observables.

ABSTRACT: Nonadiabatic molecular dynamics offers a powerful tool for studying the photochemistry of molecular systems. Key to any nonadiabatic molecular dynamics simulation is the definition of its initial conditions (ICs), ideally representing the initial molecular quantum state of the system of interest. In this work, we provide a detailed analysis of how ICs may influence the calculation of experimental observables by focusing on the photochemistry of methylhydroperoxide (MHP), the simplest and most abundant organic peroxide in our atmosphere. We investigate the outcome of trajectory surface hopping simulations for distinct sets of ICs sampled from different approximate quantum distributions, namely harmonic Wigner functions and ab initio molecular dynamics using a quantum thermostat (QT).

SUBMITTER: Prlj A 

PROVIDER: S-EPMC10493954 | biostudies-literature | 2023 Sep

REPOSITORIES: biostudies-literature