ULTRAFAST INFRARED PUMP-PROBE SPECTROSCOPY OF WATER - A THEORETICAL DESCRIPTION
ULTRAFAST INFRARED PUMP-PROBE SPECTROSCOPY OF WATER - A THEORETICAL DESCRIPTION
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DOI：
10.1063/1.467441
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发表时间：
1994-09-15
影响因子：
4.4
通讯作者：
LEICKNAM, JC
中科院分区：
文献类型：
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作者：
BRATOS, S;LEICKNAM, JC
发展了一种理论来描述最近在水中的红外泵浦-探测实验。这一理论是一种统计理论，类似于前面解释紫外线和可见光光谱的理论。利用系统电偶极矩和入射电场的四次关联函数分析了所涉及的非线性光学过程。给出了瞬时红外信号的解析表达式。观察到的光谱特性归因于初始泵浦准备状态的逐渐热化。对观测到的谱带的亚结构进行了解释。本实验探索了不同长度氢键相互转化的动力学。
A theory is developed to describe a recent infrared pump-probe experiment in water. This theory is a statistical theory, similar to those elaborated earlier to interpret ultraviolet and visible spectra. Nonlinear optical processes involved are analyzed in terms of four-time correlation functions of the electric dipole moment of the system and of the incident electric fields, respectively. An analytical expression for the transient infrared signal is presented. The observed spectral characteristics are attributed to a gradual thermalization of the initial, pump-prepared state. The substructure of the observed bands is interpreted. This experiment probes the kinetics of conversion of H-bonds of different lengths into each other.