Multidimensional spectroscopic measurements on single molecules and ensembles taking advantage of broadband shaped pulses

化学系的化学结构、动力学和机理(CSDM-A)项目获得该奖项，资助密歇根州立大学的Marcos Dantus教授开展研究溶液中光激发分子的早期动力学的实验工作。丹图斯教授和他的团队正在推动这项技术的发展，以便能够对溶液中的单分子进行测量。这类研究的最终目的是更好地了解电子激发的分子通过反应或弛豫失去能量的方式。参与这一项目的研究生和本科生将接受世界级的激光和光学培训，其中许多人来自代表性不足的群体。丹图斯教授研究的一个独特方面是，他在NSF支持下所做的许多创新都在市场上产生了新产品。学生研究人员将从与这位创业导师的合作中受益。为了帮助培养下一代科学家，丹图斯教授将继续与本科生和高中生一起在他的实验室进行研究。马科斯·丹图斯教授和他的研究小组将使用成形的飞秒激光脉冲来探测溶液中光激发分子的早期动力学。这项研究的最终目标是回答以下问题：(1)分子间(溶剂化)和分子内脱相是否可以解耦？以及(2)在没有系综平均的情况下，分子的电子相干性能保持多久？这项实验工作将受益于与著名理论家Shaul Mukamel教授在这一研究领域的合作。这项工作将导致基于单个宽带整形激光脉冲的新的多维光谱测量，其结果的理论和数值模拟将促进我们对激光-分子相互作用的了解和预测。这项研究将产生关于相干时间尺度的知识，这对于控制光化学过程和理解自然和合成光合作用系统是有价值的。

With this award, the Chemical Structure, Dynamics and Mechanisms (CSDM-A) Program of the Division of Chemistry is funding Professor Marcos Dantus of Michigan State University to conduct experimental work looking at the early-time dynamics of photoexcited molecules in solution. Professor Dantus and his group are pushing the technology to be able to make measurements of single molecules in solution. The ultimate goal of research like this is to obtain a better understanding of the ways that electronically excited molecules lose their energy through reaction or relaxation. The graduate and undergraduate students, many from underrepresented groups, working on this project will receive world-class training in lasers and optics. A unique aspect of Professor Dantus' research is that many of the innovations that he has made with NSF support have resulted in new products in the marketplace. Student researchers will benefit from working with this entrepreneurial mentor. In helping to train the next generation of scientists, Prof. Dantus will continue to work with undergraduate students as well as high school students to conduct research in his laboratory. Prof. Marcos Dantus and his research group will use shaped femtosecond laser pulses to probe the early-time dynamics of photoexcited molecules in solution. The ultimate goals of the research are to answer the questions: (1) Can intermolecular (solvation) and intramolecular dephasing be decoupled? and (2) For how long do molecules retain electronic coherence in the absence of ensemble averaging? The experimental work will benefit from a collaboration with a prominent theorist, Professor Shaul Mukamel, in this research area. This work will lead to novel multidimensional spectroscopic measurements based on a single broadband shaped laser pulse.Theory and numerical simulation of the results will advance our knowledge and predictability related to laser-molecule interactions. This study will result in knowledge about coherence timescale that can be valuable for controlling photochemical processes and understanding of natural and synthetic photosynthetic systems.