小分子在真空紫外波段从量子态到量子态的光解离动力学（英文）

Quantum State-to-State Vacuum Ultraviolet Photodissociation Dynamics of Small Molecules

本文主要描述小分子在真空紫外波段(VUV,6∽20 eV)光解离动力学的最新实验和理论研究进展.得益于基于商业化激光器的真空紫外光源技术,以及离子速度成像、高分辨氢原子-里德堡态标记-飞行时间测量和VUV-VUV泵浦-探测等方法的发展,研究人员现在可以对很多小分子在真空紫外波段的光解离动力学进行量子态到量子态层面的测量和研究.本文重点综述H2(D2, HD),CO,N2,NO,O2,H2O(D2O,HOD),CO2,N2O以及一些多原子分子在真空紫外波段光解离动力学的最新研究进展.这些小分子在真空紫外波段的光解离在天体化学以及大气化学中有着非常重要的应用.分子吸收一个VUV光子以后,通常会被直接激发到比较高的电子激发态,解离过程会涉及到多个电子态势能面之间的复杂非绝热相互作用.在实验上对解离截面等参数进行从量子态到量子态层面的精细测量对于深入了解这些复杂的势能面之间的相互作用有非常重要的意义.最近建成的大连相干光源是目前世界上唯一一台在真空紫外波段工作的自由电子激光,具有脉冲能量高、扫描范围宽(50∽150nm)等优越的性能,它的建成必将会大大促进小分子真空紫外光解离研究的发展.

The present review focused on selected, recent experimental progress of photodissociation dynamics of small molecules covering the vacuum ultraviolet (VUV) range from 6 eV to 20 eV. These advancements come about due to the available laser based VUV light sources along with the developments of advanced experimental techniques, including the velocitymap imaging (VMI), H-atom Rydberg tagging time-of-flight (HRTOF) techniques, as well as the two-color tunable VUV-VUV laser pump-probe detection method. The applications of these experimental techniques have allowed VUV photodissociation studies of many diatomic and triatomic molecules to quantum state-to-state in detail. To highlight the recent accomplishments, we have summarized the results on several important molecular species, including H2 (D2, HD), CO, N2, NO, O2, H2O (D2O, HOD), CO2, and N2O. The detailed VUV photodissociation studies of these molecules are of astrochemical and atmospheric relevance. Since molecular photodissociation initiated by VUV excitation is complex and is often governed by multiple electronic potential energy surfaces, the unraveling of the complex dissociation dynamics requires state-to-state cross section measurements. The newly constructed Dalian Coherent Light Source (DCLS), which is capable of generating coherent VUV radiation with unprecedented brightness in the range of 50-150 nm, promises to propel the photodissociation experiment to the next level.