Journal
MOLECULAR PHYSICS
Volume 119, Issue 21-22, Pages -Publisher
TAYLOR & FRANCIS LTD
DOI: 10.1080/00268976.2021.1958019
Keywords
-
Funding
- Deutsche Forschungsgemeinschaft (DFG) [KO 945/22-1]
Ask authors/readers for more resources
The spectroscopy and dynamics of the smallest Criegee intermediate CH2OO following UV excitation to the B state have been theoretically studied. Two distinct energetic regimes, distinguished based on higher resolution UV absorption spectrum, reveal the prompt dissociation in a higher-energy regime and narrow resonances in a lower-energy regime within the system. Additionally, the importance of nonadiabatic coupling effects and future steps for improved theoretical treatment are outlined.
The spectroscopy and dynamics of the smallest Criegee intermediate CH2OO following UV excitation to the B state is studied theoretically, based on multireference electronic wave functions and a quantum dynamical approach for the nuclear motion. Two interacting electronic states and two nuclear degrees of freedom are considered in the dynamical treatment. The UV absorption spectrum is found to agree very well with available experimental recordings when accounting for broadening effects due to vibrational and rotational congestion and lifetime effects. Upon higher resolution two different energetic regimes can be approximately distinguished, a higher-energy regime where the spectral envelope is broad and structureless, and dissociation is prompt, and a lower-energy regime featuring narrow resonances which are supported by the shallow well occurring at intermediate O-O distances, and decay by tunnelling to the repulsive outer part of the potential energy surface. The importance of nonadiabatic coupling effects is pointed out and future steps for an improved theoretical treatment are outlined. [GRAPHICS] .
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available