Site-Specific Time-Resolved Multidimensional Spectroscopy of Electron Transfer Dynamics

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In this project funded by the Chemical Structure and Dynamics Program A of the Chemistry Division, Professor Kevin Kubarych of the University of Michigan and his graduate students are developing de novo ("from scratch") proteins to study the fundamental motion of electrons. Electron transfer processes are essential to life, and they underlie many of the most pressing challenges in developing new methods to harvest energy and convert it into useful forms. The project promotes research opportunities arising from spectroscopic tools such as used in the research via a series of workshops and meetings.Professor Kubarych's research group uses advanced ultrafast laser spectroscopy methods to visualize electron transfer in real time using designed de novo metalloenzyme scaffolds. The combined synthetic and spectroscopic approach offers the flexibility to change the location of the electron donor and acceptor, and to add accelerating bridging side chains. Complementing this macromolecular design strategy is a spectroscopic toolset based on multidimensional spectroscopy that has been developed in the Kubarych lab. The project also uses a collaborative NSF-funded facility, the Laboratory for Ultrafast Multidimensional Optical Spectroscopy (LUMOS). LUMOS is being developed to track electron transfer and other phototriggered reactions from femtoseconds to seconds at wavelengths ranging from the UV and visible to the infrared. This extremely broad temporal and frequency range is essential to monitor changes in structure and dynamics as the charge moves through the engineered protein.