Linear and Nonlinear Resonance Raman Studies of Photodissociation

在实验物理化学计划的支持下，齐格勒教授正在开发和使用新的拉曼光谱技术，以足够的分辨率来研究小多原子分子中的光解过程的动态，以检查单个的旋转-振动能级。先前开发的旋转共振拉曼技术被用来测量短寿命（20飞秒至5皮秒）准束缚激发态能级的振转量子特定寿命。共振超喇曼是扩展的工作，解离分子激发态的真空紫外接近通过双光子过程与近紫外光子。计划的工作还包括使用共振相干反斯托克斯拉曼光谱（汽车），以实现更大的旋转量子分辨率，并允许更大的分子的研究。为了控制和预测化学反应的过程，人们必须在分子水平上理解反应动力学作为空间和时间的函数。这项实验和理论研究将侧重于扩大我们对光解过程的详细理解，即吸收光后分子的分裂。在这项工作中的光解过程将在几种情况下检查的依赖性的结果上的初始能量状态的吸收物种。

With support from the Experimental Physical Chemistry Program, Professor Ziegler is developing and using novel Raman spectroscopic techniques to investigate the dynamics of photodissociation processes in small polyatomic molecules at a resolution sufficient to examine individual rotational- vibrational levels. Previously developed rotational resonance Raman techniques are being used to measure rovibrational quantum specific lifetimes of short-lived (20 femtoseconds to 5 picoseconds) quasi-bound excited state levels. Resonance hyper-Raman is extending the work to dissociative molecular excited states in the vuv accessible via two-photon processes with near-uv photons. Planned work also includes the use of resonant Coherent Anti-Stokes Raman Spectroscopy (CARS) to achieve greater rotational quantum resolution and allow the study of larger molecules. %%% In order to control and predict the course of chemical reactions, one must understand the dynamics of reactions on a molecular level as a function of both space and time. This experimental and theoretical study will focus on expanding our detailed understanding of the process of photodissociation, that is, the breaking apart of a molecule after the absorption of light. In this work the photodissociation process will be examined in several cases for the dependence of the outcome on the initial energy state of the absorbing species.