School of Chemistry, University of Bristol, Cantock's Close, Bristol BS8 1TS, UK.
Phys Chem Chem Phys. 2010 Aug 28;12(32):9129-43. doi: 10.1039/c001233e. Epub 2010 May 6.
The experimental technique of velocity map imaging (VMI) enables measurements to be made of the dynamics of chemical reactions that are providing unprecedented insights about reactive scattering. This perspective article illustrates how VMI, in combination with crossed-molecular beam, dual-beam or photo-initiated (Photoloc) methods, can reveal correlated information on the vibrational quantum states populated in the two products of a reaction, and the angular scattering of products (the differential cross section) formed in specific rotational and vibrational levels. Reactions studied by VMI techniques are being extended to those of polyatomic molecules or radicals, and of molecular ions. Subtle quantum-mechanical effects in bimolecular reactions can provide distinct signatures in the velocity map images, and are exemplified here by non-adiabatic dynamics on coupled potential energy surfaces, and by experimental evidence for scattering resonances.
速度成像(VMI)实验技术能够对化学反应动力学进行测量,为反应散射提供了前所未有的深入了解。本文通过实例说明了 VMI 如何与交叉分子束、双束或光引发(Photoloc)方法相结合,揭示反应的两个产物中振动量子态的相关信息,以及在特定转动和振动能级下形成的产物的角散射(微分截面)。VMI 技术研究的反应正扩展到多原子分子或自由基,以及分子离子。双分子反应中的微妙量子力学效应可以在速度成像中提供明显的特征,本文通过耦合势能表面上的非绝热动力学以及散射共振的实验证据对此进行了举例说明。