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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Doppler-Resolved Kinetics of Saturation Recovery
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Doppler-Resolved Kinetics of Saturation Recovery

机译：多普勒解析的饱和恢复动力学

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摘要

Frequency-modulated laser transient absorption has been used to monitor the ground-state rotational energy-transfer rates of CN radicals in a double-resonance, depletion recovery experiment. When a pulsed laser is used to burn a hole in the equilibrium ground-state population of one rotational state without velocity selection, the population recovery rate is found to depend strongly on the Doppler detuning of a narrow-band probe laser. Similar effects should be apparent for any relaxation rate process that competes effectively with velocity randomization. Alternative methods of extracting thermal rate constants in the presence of these non-thermal conditions are evaluated. Total recovery rate constants, analogous to total removal rate constants in an experiment preparing a single initial rotational level, are in good agreement with quantum scattering calculations, but are slower than previously reported experiments and show qualitatively different rotational state dependence between Ar and He collision partners. Quasi-classical trajectory studies confirm that the differing rotational state dependence is primarily a kinematic effect.
机译：调频激光瞬态吸收已用于在双共振耗尽恢复实验中监测CN自由基的基态旋转能量转移速率。当使用脉冲激光在不进行速度选择的情况下在一个旋转状态的平衡基态种群中燃烧洞时，发现种群恢复率在很大程度上取决于窄带探测激光器的多普勒失谐。对于与速度随机化有效竞争的任何松弛速率过程，类似的效果也应显而易见。评估了在这些非热条件下提取热速率常数的替代方法。总回收率常数类似于准备单个初始旋转能级的实验中的总去除率常数，与量子散射计算非常吻合，但比以前报道的实验要慢，并且显示出Ar和He碰撞伙伴之间的旋转态依赖性在质上有差异。准经典轨迹研究证实，不同的旋转状态依赖性主要是运动学上的影响。

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