Using a multistate Mapping Approach to Surface Hopping to predict the Ultrafast Electron Diffraction signal of gas-phase cyclobutanone
arxiv(2024)
摘要
Using the recently developed multistate mapping approach to surface hopping
(multistate MASH) method combined with SA(3)-CASSCF(12,12)/aug-cc-pVDZ
electronic structure calculations, the gas-phase isotropic ultrafast electron
diffraction (UED) of cyclobutanone is predicted and analyzed. After excitation
into the n-3s Rydberg state (S_2), cyclobutanone can relax through two
S_2/S_1 conical intersections, one characterized by compression of the
CO bond, the other by dissociation of the α-CC bond.
Subsequent transfer into the ground state (S_0) is then achieved via two
additional S_1/S_0 conical intersections that lead to three reaction
pathways: α ring-opening, ethene/ketene production, and CO
liberation. The isotropic gas-phase UED signal is predicted from the multistate
MASH simulations, allowing for a direct comparison to experimental data. This
work, which is a contribution to the cyclobutanone prediction challenge,
facilitates the identification of the main photoproducts in the UED signal and
thereby emphasizes the importance of dynamics simulations for the
interpretation of ultrafast experiments.
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