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

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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.