1.
J Chem Phys
; 160(16)2024 Apr 28.
Artigo
em Inglês
| MEDLINE
| ID: mdl-38686819
RESUMO
We study the ultrafast time evolution of cyclobutanone excited to the singlet n â Rydberg state through non-adiabatic surface-hopping simulationsperformed at extended multi-state complete active space second-order perturbation (XMS-CASPT2) level of theory. These dynamics predict relaxation to the ground-state with a timescale of 822 ± 45 fs with minimal involvement of the triplets. The major relaxation path to the ground-state involves a three-state degeneracy region and leads to a variety of fragmented photoproducts. We simulate the resulting time-resolved electron-diffraction spectra, which track the relaxation of the excited state and the formation of various photoproducts in the ground state.