Optical Control of Condensed Phase Reaction Dynamics

在这个由化学学部实验物理化学项目资助的奖项中，密歇根大学的Roseanne Sension教授和她的博士后研究员以及研究生计划进行旨在影响凝聚相分子动力学和化学反应性的实验，并通过学习算法方法确定有效的脉冲形状。这些研究的总体目标集中在将复杂的反应动力学观察与直接或间接控制化学反应的能力联系起来。提出了5个特定的体系用于研究：1)顺式二苯乙烯反应激发态支化的控制，2)溶液中光解通道的控制，3)嘧啶DNA碱基激发态支化的控制，4)1,3-环己二烯开环反应，5)维生素D原开环反应。技术，如紫外线（UV）脉冲整形，激发态测量，理论计算，和多光子激光激发将被采用。这项工作的性质是现代光学技术的最前沿，并使学生接触到化学物理学和光学物理学的最新研究。学生和其他研究人员将有机会获得先进的激光脉冲产生技术。与教育的整合将包括增加计算化学课程，包括在超快激光实验中观察到的化学动力学的建模和模拟。

In this award, funded by the Experimental Physical Chemistry Program of the Division of Chemistry, Professor Roseanne Sension of the University of Michigan along with her post-doctoral fellows and graduate students plan to perform experiments aimed at influencing both condensed phase molecular dynamics & chemical reactivity along with the identification of effective pulse shapes through learning algorithm approaches. The overarching goal of these studies is focused on linking sophisticated observation of reaction dynamics with the ability to control chemical reactions either directly or indirectly. Five specific systems are proposed for study: 1) Control of Reactive Excited State Branching in Cis-Stilbene, 2) Control of Photodissociation Channels in Solution Phase, 3) Control of Excited State Branching in Pyrimidine DNA Bases, 4) 1,3-Cyclohexadiene Ring-Opening Reaction, and 5) The Pro-Vitamin D Ring-Opening Reaction. Techniques such as ultraviolet (UV) pulse shaping, excited state measurements, theoretical calculations, and multi-photon laser excitation will be employed.The nature of this work is at the forefront of modern optical techniques and exposes students to state-of-the-art research in chemical physics and optical physics. Students and other research associates will have access to advanced laser pulse generation techniques. Integration with education will include augmenting the computational chemistry curriculum to include modeling and simulation of the chemical dynamics observed in ultrafast laser experiments.