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化学学报
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化学学报 ›› 2006, Vol. 64 ›› Issue (18): 1865-1870. 上一篇    下一篇

研究论文

超快速反应荧光亏蚀谱微观动力学理论

曹宵鸣, 陆靖*, 范康年   

  1. (复旦大学化学系 上海市分子催化与创新材料重点实验室 理论化学物理中心 上海 200433)
  • 投稿日期:2005-11-01 修回日期:2006-05-16 发布日期:2006-09-28
  • 通讯作者: 陆靖

Dynamical Theory of Fluorescence Depletion in Ultrafast Reaction

CAO Xiao-Ming; LU Jing*; FAN Kang-Nian   

  1. (Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Material, Centre for Theoretical Chemical Physics, Fudan University, Shanghai 200433)
  • Received:2005-11-01 Revised:2006-05-16 Published:2006-09-28
  • Contact: LU Jing

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用超短脉冲激发动力学光谱理论在两电子体系下模拟了飞秒时间分辨的荧光亏蚀谱, 再现了实验中所得荧光亏蚀谱的双指数衰减和凹陷两种现象, 这两种现象分别是由于探测脉冲使电子激发态上振动基态和较高振动态的分子受激发射而产生的.

关键词: 荧光亏蚀谱, 飞秒脉冲, 振动弛豫

The dynamical theory of spectroscopy with ultrashort pulse excitation is developed to simulate the femtosecond time-resolved fluorescence depletion with the bielectron system. The double exponential decay curve and hollow of fluorescence depletion on the experiment are recurred. The microdynamical causation of these is explained. It is found that the stimulated emission of excited molecules on vibrational ground and higher vibrational level by probe pulse respectively leads to the double exponential decay curve and the hollow of fluorescence depletion.

Key words: fluorescence depletion, femtosecond pulse, vibrational relaxation