Multidimensional Femtosecond Studies of Chemical Reaction Dynamics

在这个由化学系实验物理化学计划资助的奖项中，科罗拉多大学的大卫乔纳斯教授将利用二维光谱学研究光激发脉冲的相位对分子系统动力学控制的作用。 具体而言，将审查三大领域。 首先，将测试用于去除强吸收样品的飞秒2D光谱中的传播失真的方法。 然后，二维光谱将用于探测电子通过圆锥形交叉点从一个轨道到另一个轨道的运动速度，这是一种重要的机制，有助于化学反应过程中的键合变化。 最后，成形的飞秒脉冲将被用来确定弱激光场的相位控制是否可以修改凝聚相中的光驱动反应的结果，而不改变光的强度spectrum. Two-dimensional Fourier transform infrared and optical spectroscopy is a relatively new technique that has potential to become an important analytical tool for measuring of new molecular properties. 就像在2D-NMR中一样，类似的2D光学和红外傅里叶变换光谱以二维模式显示特征光谱，其揭示相邻键及其相对几何形状。 特别是，这些研究将有助于建立目前应用于一系列科学问题的多维电子光谱类型背后的理论。 参加本研究的研究生和博士后研究人员获得新的知识和技能，为深造或进入科学/技术就业市场做准备。

In this award funded by the Experimental Physical Chemistry Program of the Division of Chemistry, Professor David Jonas of University of Colorado will use two-dimensional spectroscopy to study the role of the phase of an optical excitation pulse on the dynamical control of molecular systems. In particular, three broad areas will be examined. First, an approach for removing propagation distortions in femtosecond 2D spectra of strongly absorbing samples will be tested. Two-dimensional spectroscopy will then be used to probe the speed of electronic motion from one orbital to another via conical intersections, which are an important mechanism that facilitates bonding changes during chemical reactions. Finally, shaped femtosecond pulses will be used to determine whether phase control of weak laser fields can modify the outcome of light-driven reactions in condensed phases without changing the intensity spectrum of the light.Two-dimensional Fourier transform infrared and optical spectroscopy is a relatively new technique that has the potential of becoming an important analytical tool for the measurement of new molecular properties. Just as in 2D-NMR, analogous 2D optical and infrared Fourier transform spectra show characteristic spectra in two-dimensional patterns that reveal adjacent bonds and their relative geometry. In particular, these studies will help establish the theory behind the types of multidimensional electronic spectroscopies currently being applied to a range of scientific problems. Graduate students and postdoctoral research associates who participate in this research acquire new knowledge and skills in preparation for advanced studies or entrance into the scientific/technological job market.