期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 8, 期 5, 页码 1019-1024出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.6b02897
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资金
- National Natural Science Foundation of China [21522302, 21520102005, 21421003, 21590801]
- Recruitment Program of Global Youth Experts
- Fundamental Research Funds for Central Universities
We have employed combined electronic structure calculations and nonadiabatic dynamics simulations to study the S-1 radiationless deactivation mechanism of pyrazole. In terms of MS-CASPT2 computed results, we propose that the (1)pi sigma* state-driven nonadiabatic N-N dissociation is a major relaxation path; the ring-puckering deformation path as well as the (1)pi sigma* state-driven N-H dissociation are less favorable. This excited-state decay mechanism is supported by MS-CASPT2 nonadiabatic dynamics simulations. The present study demonstrates that pyrazole has a different excited-state radiationless deactivation mechanism compared with its structural isomer imidazole, in which the (1)pi sigma* state driven nonadiabatic N-H dissociation plays a more important role. However, such a channel is suppressed in pyrazole; instead, the (1)pi sigma* state driven nonadiabatic N-N dissociation is dominant.
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