Time-resolved broadband Raman spectroscopies: A unified six-wave-mixing representation
Time-resolved broadband Raman spectroscopies: A unified six-wave-mixing representation
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DOI：
10.1063/1.4821228
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发表时间：
2013-09-28
影响因子：
4.4
通讯作者：
Mukamel, Shaul
中科院分区：
文献类型：
--
作者：
Dorfman, Konstantin E.;Fingerhut, Benjamin P.;Mukamel, Shaul
激发态分子振动动力学可以通过电子非共振拉曼过程研究，该过程由相对于光化脉冲具有可变延迟的探测脉冲引起。我们建立了几个变种的技术，涉及无论是自发或受激拉曼检测和不同的脉冲配置之间的连接。通过在频域中使用回路图，我们表明，所有的信号可以被描述为六波混频依赖于相同的四点分子相关函数，涉及两个过渡偶极子和两个极化率，并伴随着不同的门。随机两态跳跃模型的模拟说明了实验观察到的吸收和色散特性的起源。(C)2013 AIP Publishing LLC.
Excited-state vibrational dynamics in molecules can be studied by an electronically off-resonant Raman process induced by a probe pulse with variable delay with respect to an actinic pulse. We establish the connection between several variants of the technique that involve either spontaneous or stimulated Raman detection and different pulse configurations. By using loop diagrams in the frequency domain, we show that all signals can be described as six wave mixing which depend on the same four point molecular correlation functions involving two transition dipoles and two polarizabilities and accompanied by a different gating. Simulations for the stochastic two-state-jump model illustrate the origin of the absorptive and dispersive features observed experimentally. (C) 2013 AIP Publishing LLC.