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Understanding spectroscopic probes of entangled electronic and nuclear dynamics in electronic excitation transfer

We have developed a general framework for calculating and interpreting multi-dimensional electronic spectroscopy signals in terms of the wave-packet-shaping, amplitude-transferring effects of femtosecond laser pulses on time-dependent molecular states. I'll describe the treatment of two-dimensional wave-packet interferometry (WPI) experiments on an electronic energy-transfer (EET) system as quantum yield-weighted sums of contributing overlaps between multi-pulse wave packets. Example calculations will be presented for the cases of a spatially oriented, weakly- or strongly-coupled EET dimer. In a recent application of these ideas, I'll outline a proposed WPI-based strategy for directly tracking the evolution of inter-site or inter-exciton coherence in an excitation-transfer dimer.