The fascinating field of photoinduced charge-transfer holds many open questions:  Controlling charge-recombination? Mechanisms of energy dissipation? The role of specific vibrations and vibrational/vibronic coupling?We design Donor-spacer-Acceptor assemblies of transition-metal chromophores with lifetimes of charge-separated state from picoseconds to sub-microseconds. Ultrafast transient absorption, time-resolved IR and transient 2DIR spectroscopies reveal the role of specific vibrations in the intra-molecular charge-transfer, through the mode-connectivity patterns over large distances. Three-pulse [UV-pump/IR-pump/IR-probe] studies demonstrate exciting possibilities of modulating molecular photoreactivity by mode-specific vibrational perturbation.

Ultrafast photoinduced charge-separation in molecular systems: Time-resolved IR, transient 2DIR, and controlling the rates and the pathways by vibrational perturbation

245th National Meeting (2013)

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