Isomerization Dynamics of 1,1'-Diethyl-4,4'-Cyanine (1144C) Studied by Different Third-Order Nonlinear Spectroscopic Measurements

Qing-Hua Xu; Graham R. Fleming

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Isomerization Dynamics of 1,1'-Diethyl-4,4'-Cyanine (1144C) Studied by Different Third-Order Nonlinear Spectroscopic Measurements

机译：不同三阶非线性光谱测量研究1,1'-二乙基-4,4'-花菁（1144C）的异构化动力学

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The isomerization of 1,1'-diethyl-4,4'-cyanine (1144C) in two solvents, ethanol and hexanol, was studied by three different third-order four-wave mixing techniques: three-pulse photon echo peak shift (3PEPS), transient grating (TG), and pump-probe (PP) to provide complimentary information on different aspects of the reaction dynamics. A double-sided Feynman diagram analysis was used to assist in the formulation of the kinetic behavior in the TG and AP signals. The ground-state recovery process can be described as a single exponential process which is dominated by the bond-twisting motion on the excited-state surface. The rate is strongly viscosity and temperature dependent. A larger yield of the isomer is obtained in less viscous solvents or with greater excess excitation energy. Apparently, contradictory wavelength-dependent decay behavior was found in the TG and PP signals. This can be understood by considering the different real and imaginary contributions to the signals from hot ground-state absorption and its subsequent recovery tot he equilibrated state and from the product state.

机译：通过三种不同的三阶四波混合技术研究了1,1'-二乙基-4,4'-花菁（1144C）在两种溶剂乙醇和己醇中的异构化：三脉冲光子回波峰位移（3PEPS ），瞬态光栅（TG）和泵浦探针（PP），以提供有关反应动力学不同方面的补充信息。双面费恩曼图分析用于协助制定TG和AP信号的动力学行为。基态恢复过程可以描述为单个指数过程，该过程主要受激发态表面上的键扭转运动影响。该速率强烈取决于粘度和温度。在粘度较低的溶剂中或在较大的过量激发能下，可获得较高的异构体收率。显然，在TG和PP信号中发现了与波长相关的衰减行为。通过考虑热基态吸收及其从平衡态到产品态的后续恢复对信号的不同实部和虚部贡献，可以理解这一点。

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《The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory》 |2001年第45期|共9页
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Qing-Hua Xu; Graham R. Fleming;
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中图分类物理化学（理论化学）、化学物理学;
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1. Isomerization Dynamics of 1,1'-Diethyl-4,4'-Cyanine (1144C) Studied by Different Third-Order Nonlinear Spectroscopic Measurements [J] . Qing-Hua Xu, Graham R. Fleming The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory . 2001,第45期

机译：不同三阶非线性光谱测量研究1,1'-二乙基-4,4'-花菁（1144C）的异构化动力学
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Isomerization Dynamics of 1,1'-Diethyl-4,4'-Cyanine (1144C) Studied by Different Third-Order Nonlinear Spectroscopic Measurements

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