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Communication: Uncovering correlated vibrational cooling and electron transfer dynamics with multidimensional spectroscopy
P. Hamm and M. T. Zanni, Concepts and Methods of 2D Infrared Spectroscopy (Cambridge University Press, Cambridge, 2011).
C. Reichardt and T. Welton, Solvents and Solvent Effects in Organic Chemistry, 4th ed. (Wiley-VCH, Weinheim, 2011).
S. Mukamel, Principles of Nonlinear Optical Spectroscopy (Oxford University Press, New York, 1995).
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Analogues of 2D photon echo methods in which two population times are sampled have recently been used to expose heterogeneity in chemical kinetics. In this work, the two population times sampled for a transition metal complex are transformed into a 2D rate spectrum using the maximum entropy method. The 2D rate spectrum suggests heterogeneity in the vibrational cooling (VC) rate within the ensemble. In addition, a cross peak associated with VC and back electron transfer (BET) dynamics reveals correlation between the two processes. We hypothesize that an increase in the strength of solute-solvent interactions, which accelerates VC, drives the system toward the activationless regime of BET.
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