The Simulation of Femtosecond VUV Time-Resolved Molecular Spectroscopy

Abstract

Femtosecond vacuum-ultraviolet (VUV) laser pulses enable the interrogation of molecules in their electronically excited states on the timescale of nuclear motion. The present study focuses on the simulation of these experiments using electronic structure calculations and nuclear wavepacket dynamics propagations. The simulation of the evolution of the wavepacket enables a calculation of spectroscopic observables using rigorous quantum mechanical approaches. This approach has been applied to simulate the VUV time-resolved photoelectron spectroscopy (TRPES) spectra of cyclopropane (C₃H₆) and nitromethane (CH₃NO₂).