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羟基自由基与氦气和氩气的非弹性散射的速度成像研究。

Inelastic scattering of hydroxyl radicals with helium and argon by velocity-map imaging.

机构信息

Institute for Molecules and Materials, Radboud University Nijmegen, Heijendaalseweg 135, 6525 ED Nijmegen, The Netherlands.

出版信息

Nat Chem. 2012 Dec;4(12):985-9. doi: 10.1038/nchem.1480. Epub 2012 Oct 28.

Abstract

The hydroxyl radical (OH) is one of the most interesting molecules in molecular dynamics. In particular, inelastic collisions of free radicals such as OH are profoundly important in environments ranging from combustion to astrochemistry. However, measuring the velocities of OH molecules in specific internal quantum states has proven to be very difficult. A method that can provide this important information is velocity-map imaging. Although this technique is very widely applicable in principle, it does require a sensitive and selective laser-ionization scheme. Here we show that, under the right conditions, velocity-map imaging can be applied to the study of the inelastic scattering of OH using crossed-molecular-beam methods. We measure fully quantum-state-specified product angular distributions for OH collisions with helium and argon. The agreement between exact close-coupling quantum scattering calculations on ab initio potential energy surfaces and experimental data is generally very satisfactory, except for scattering in the most forward directions.

摘要

羟基自由基(OH)是分子动力学中最有趣的分子之一。特别是,在从燃烧到天体化学的各种环境中,自由基如 OH 的非弹性碰撞具有非常重要的意义。然而,测量特定内部量子态下的 OH 分子速度已被证明非常困难。一种可以提供此重要信息的方法是速度图成像。尽管该技术在原理上具有非常广泛的适用性,但它确实需要灵敏和选择性的激光电离方案。在这里,我们表明,在适当的条件下,速度图成像可以应用于使用交叉分子束方法研究 OH 的非弹性散射。我们测量了 OH 与氦和氩碰撞的完全量子态指定产物角分布。基于从头算势能面的精确密耦量子散射计算与实验数据之间的一致性通常非常令人满意,除了最前向散射方向。

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