Verlet Jan R R, Horke Daniel A, Chatterley Adam S
Department of Chemistry, University of Durham, Durham DH1 3LE, UK.
Phys Chem Chem Phys. 2014 Aug 7;16(29):15043-52. doi: 10.1039/c4cp01667j. Epub 2014 Jun 23.
Many properties of isolated multiply-charged anions (MCAs) are dictated by the strong intra-molecular Coulomb interactions that are present. The most striking property of MCAs is a long-range repulsive Coulomb barrier (RCB) that arises from the repulsive interaction between an electron and an anion which must be overcome to form a MCA. Excited states provide a route to probing this RCB and the focus of this Perspective is on recent photoelectron experiments, including angularly and temporally resolved, that have provided detailed physical insight into the RCB surfaces, their anisotropy, and their use to monitor molecular dynamics in real-time. An outlook provides some future prospects that studies on MCAs provide in terms of monitoring structural, charge-migration, and solvation dynamics.
孤立的多电荷阴离子（MCA）的许多性质由其内部存在的强库仑相互作用决定。MCA最显著的性质是长程排斥库仑势垒（RCB），它源于电子与阴离子之间的排斥相互作用，形成MCA时必须克服这种相互作用。激发态为探测这种RCB提供了一条途径，本文的重点是近期的光电子实验，包括角度分辨和时间分辨实验，这些实验对RCB表面、其各向异性以及实时监测分子动力学的用途提供了详细的物理见解。展望部分给出了MCA研究在监测结构、电荷迁移和溶剂化动力学方面的一些未来前景。
