Multidimensional Femtosecond Studies of Chemical Reaction Dynamics

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In this project funded by the Chemical Measurement and Imaging program of the Chemistry Division, Professor David Jonas of the University of Colorado at Boulder is developing two-dimensional femtosecond spectroscopy as a tool for measuring the motions of electrons in ultrafast chemical reactions. The factors controlling efficient transport of charge and energy at the molecular level are not understood, but are important for ultrafast chemical reactions in both natural photosynthesis and light harvesting technologies. The project involves an international scientific collaboration to implement the two-dimensional spectroscopy technique developed at the University of Colorado over ultra-broad frequency ranges using pulsed lasers developed at the Institute of Photonic Sciences in Spain.This project focuses on a two-color 2D electronic spectroscopy in which visible pulses excite molecules to their first excited electronic state and short-wave infrared pulses detect electronic absorption. This approach uniquely isolates dynamics on the excited state, which can involve non-adiabatic coupling between vibrational and electronic motions. The project aims to experimentally develop two-dimensional spectroscopy in the short-wave infrared region of the spectrum and use this capability to improve our understanding of carotenoid dynamics and photosynthetic energy transfer. The broader impacts of this work include scientific training of a graduate student and a postdoctoral researcher, their exposure to the scientific environment in the European Union, the development of new techniques for measuring electronic dynamics, and potential societal benefits from technologies based on an understanding of the most efficient energy harvesting reactions.