Experimental Probes of Nonadiabatic Dynamics and Novel Reaction Pathways in Polyatomic Molecules

在这个由化学部门化学结构、动力学和机制项目资助的项目中，韦恩州立大学的教授将使用对产品的电子和自旋角动量敏感的激光技术对多原子分子的解离进行研究。这些发现可以用来揭示这些分离事件的详细动力学。提出的工作的一个关键方面是开发一种有效检测氢原子光碎片中电子自旋极化的方法，这是许多多原子分子解离的主要产物。提出的研究的第二个方面是控制在甲醛和乙醛分解中发现的新型“漫游自由基”反应机制的策略。拟议工作的更广泛影响包括开发一种新的高分辨率图像采集系统，该系统将免费分发给其他团体。此外，在离子成像、激光光谱学和数据分析方法方面招收和培养多样化的本科生、研究生和博士后是该小组活动的一个核心方面。光激发分子分解的一个重要问题是在解离过程中遇到的电子态的顺序，以及它们影响最终结果的方式。这个问题直接关系到许多不同的领域，从太阳能捕获到视觉到大气化学，几乎所有分子与光相互作用的地方。

In this project funded by the Chemical Structure, Dynamics and Mechanisms Program of the Chemistry Division, Professor Suits of Wayne State University will conduct investigations of the dissociation of polyatomic molecules using laser techniques that are sensitive to the electronic and spin angular momentum of the products. The findings can then be used to unravel the detailed dynamics of these dissociation events. A key aspect of the proposed work is development of an approach for efficient detection of electron spin polarization in hydrogen atom photo-fragments, a principal product of the dissociation of a great many polyatomic molecules. A second aspect of the proposed studies is a strategy to control the novel "roaming radical" reaction mechanism identified in formaldehyde and acetaldehyde decomposition. Broader impacts of the proposed work include development of a new high-resolution image acquisition system that will be freely distributed to other groups. In addition, recruitment and training of a diverse group of undergraduate students, graduate students and post-docs in methods in ion imaging, laser spectroscopy and data analysis is a core aspect of the group activity.An important question in the decomposition of photoexcited molecules is the sequence of electronic states that are encountered in the course of dissociation, and the ways in which they influence the final outcome. This question has direct bearing in many diverse areas from solar energy capture to vision to atmospheric chemistry: almost anywhere that molecules interact with light.