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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Highly Selective Relaxation of the OH Stretching Overtones in Isolated HDO Molecules Observed by Infrared Pump-Repump-Probe Spectroscopy
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Highly Selective Relaxation of the OH Stretching Overtones in Isolated HDO Molecules Observed by Infrared Pump-Repump-Probe Spectroscopy

机译：红外泵-泵浦-探针光谱法观察到的分离的HDO分子中OH拉伸泛音的高度选择性弛豫。

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摘要

A quantitative investigation of the relaxation dynamics of higher-lying vibrational states is afforded by a novel method of infrared pump-repump-probe spectroscopy. The technique is used to study the dynamics of OH stretching overtones in NaClO4 center dot HDO monohydrate. We observe a continuous decrease of the energy separation for the first four states, i.e. nu(01), = 3575 cm(-1), nu(12) = 3370 cm(-1), and nu(23) = 3170 cm(-1), respectively. The population lifetime of the first excited state is 7.2 ps, while the one of the second excited state is largely reduced to 1.4 ps. The relaxation of the v = 2 state proceeds nearly quantitatively to the v = 1 state. The new information on the OH stretching overtones demands improved theoretical potentials and modeling of the H bond interactions. This work shows the potential of the new technique for the precise study of complex vibrational relaxation pathways.
机译：通过红外泵-泵浦-探针光谱学的新方法，可以对较高振动态的弛豫动力学进行定量研究。该技术用于研究NaClO4中心点HDO一水合物中OH拉伸泛音的动力学。我们观察到前四个状态的能量分离持续减小，即nu（01）= 3575 cm（-1），nu（12）= 3370 cm（-1）和nu（23）= 3170 cm（ -1）。第一激发态的填充寿命为7.2 ps，而第二激发态的填充寿命大大降低至1.4 ps。 v = 2状态的弛豫几​​乎定量地进行到v = 1状态。有关OH拉伸泛音的新信息要求改进理论势能和H键相互作用的建模。这项工作表明了新技术对复杂的振动弛豫路径进行精确研究的潜力。

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