Coordinated Studies of the Reaction Dynamics for Isolated and Solvated Molecules

在这个由化学部实验物理化学项目资助的项目中，弗吉尼亚大学的Brooks Pate教授将研究分离分子的反应动力学以及溶剂化改变这种内在行为的方式。将开发一种新的超快振动光谱实验设计。通过结合气相和溶液相分子光谱的最先进的实验技术，这项工作连接了物理化学的两个主要领域：分子内动力学和溶液化学。该项目的一个主要部分是研究溶剂如何影响激光脉冲传递给系统的分子内振动相干性。这些实验将测试通过红外脉冲序列操纵分离分子的振动运动和结构的能力。通过在溶液中进行的实验，将有可能确定量子操纵所需的相干性是否得以保留。该项目的第二个目标是开发一种新的光谱仪，用于使用动态旋转光谱（DRS）测量反应动力学。该项目的仪器开发部分将广泛影响科学和技术的几个领域，如燃烧动力学领域的应用，测量分子几何变化动力学的新方法，以及通过控制量子动力学来研究操纵分子性质的能力的新工具。这项工作在生物物理化学和纳米科学领域具有潜在的应用前景。参与这项研究的学生将在设计、建造和测试新的测量设备方面获得宝贵的经验。学生还将接受时域和频域光谱学基本概念的强化训练，使他们能够欣赏这些互补技术的相对优势。

In this project, funded by the Experimental Physical Chemistry Program of the Chemistry Division, Prof. Brooks Pate of the University of Virginia will investigate the reaction dynamics of isolated molecules and the way that solvation changes this intrinsic behavior. A new experimental design for ultrafast vibrational spectroscopy will be developed. By combining state-of-the-art experimental techniques for gas and solution phase molecular spectroscopy, this work bridges two of the major fields of physical chemistry: intramolecular dynamics and solution chemistry. A major part of the project is to examine how the solvent affects intramolecular vibrational coherence imparted to the system by a laser pulse. These experiments will test the ability to manipulate the vibrational motion and structure of isolated molecules through infrared (IR) pulse sequences. With experiments conducted in solution it will be possible to determine whether the coherence required for quantum manipulation is preserved. A second goal of the project is the development of a new spectrometer for measuring reaction kinetics using dynamical rotational spectroscopy (DRS).The instrumental development parts of this project will broadly impact several areas of science and technology, such as applications in the field of combustion kinetics, new approaches to measuring the kinetics of molecular geometry change, and new tools to study the ability to manipulate molecular properties through control of the quantum dynamics. This work has potential applications in the fields of biophysical chemistry and nanoscience. Students who participate in this research will gain valuable experience in the design, construction and testing of new measurement equipment. The students will also receive strong training in the fundamental concepts of both time-domain and frequency-domain spectroscopy that will allow them to appreciate the relative strengths of these complementary techniques.