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Ultrafast Decay Dynamics of the 21ππ* Electronic State of N-Methyl-2-pyridone.
Feng, Baihui; Wu, Wenping; He, Zhigang; Yang, Dongyuan; Wu, Guorong; Yang, Xueming.
Afiliación
  • Feng B; State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, Liaoning 116023, China.
  • Wu W; University of Chinese Academy of Sciences, Beijing 100049, China.
  • He Z; State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, Liaoning 116023, China.
  • Yang D; University of Chinese Academy of Sciences, Beijing 100049, China.
  • Wu G; State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, Liaoning 116023, China.
  • Yang X; State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, Liaoning 116023, China.
J Phys Chem A ; 128(19): 3840-3847, 2024 May 16.
Article en En | MEDLINE | ID: mdl-38690846
ABSTRACT
The ultrafast decay dynamics of N-methyl-2-pyridone upon excitation in the near-ultraviolet range of 261.5-227.9 nm is investigated using the femtosecond time-resolved photoelectron spectroscopy method. Irradiation at 261.5 nm prepares N-methyl-2-pyridone molecules with high vibrational levels in the 11ππ* state. The radiation-less decay to the ground state via internal conversion is suggested to be the dominant channel for the 11ππ* state with large vibrational excess energy, which is revealed by a lifetime of 1.6 ± 0.2 ps. As the pump wavelength decreases, we found that irradiation at 238.5 and 227.9 nm results in the population of the 21ππ* state. This is in agreement with the assignment of the vapor-phase UV absorption bands of N-methyl-2-pyridone. On the basis of the detailed analysis of our measured time-resolved photoelectron spectra at all pump wavelengths, we conclude that the 21ππ* state has an ultrashort lifetime of 50 ± 10 fs. In addition, the S1(11ππ*) state is subsequently populated via internal conversion and decays over a lifetime of 680-620 fs. The most probable whole deactivation pathway of the 21ππ* state is discussed. This experimental study provides new insights into the excitation energy-dependent decay dynamics of electronically excited N-methyl-2-pyridone.

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Phys Chem A Asunto de la revista: QUIMICA Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Estados Unidos

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Phys Chem A Asunto de la revista: QUIMICA Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Estados Unidos