This talk will discuss the development of femtosecond resonant multidimensional multicolor, two-dimensional electronic-vibrational (2D EV) and vibrational-electronic (2D VE) spectroscopy techniques. These experiments use a train of infrared and optical pulses to measure coupled vibrational and electronic coordinates in the system of interest. Understanding how vibronic couplings and dynamics are encoded in these new techniques will be discussed. Emphasis will be given to polarization-selectivity of the 2D EV and 2D VE techniques. Examples involving the coupling of high-frequency vibrations with charge transfer transitions in systems undergoing rapid electron and proton transfer will be discussed.

Measuring coherent vibronic couplings and dynamics with two-dimensional vibronic spectroscopy

ACS Fall 2021

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