This talk will present the development of multidimensional vibronic spectroscopies using a sequence of femtosecond infrared and optical electric fields. The experiments measure the coupling of vibrational and electronic transitions using resonant pump and probe pulses. Polarization-selective 2D vibrational-electronic (VE) spectroscopy was used to measure the vibronic couplings and angles between coupled cyanide stretching frequencies and the metal-to-metal charge transfer transition. An application of 2D and 3D electronic-vibrational spectroscopy will be described where the evolution of vibronic coherences is measured during an ultrafast intersystem crossing and subsequent triplet internal conversion in a Ru based solar cell dye. These studies describe the potential of multidimensional vibronic spectroscopies in deciphering ultrafast photochemical processes in solution.

Coherent multidimensional vibronic spectroscopies

2019 Fall National Meeting

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