A strategy is described and illustrated for quantitatively monitoring the evolution of inter-site or inter-exciton electronic coherence in weakly or strongly coupled excitation-transfer dimers, respectively, using ultrafast two-dimensional wave-packet interferometry. Turning to an equilateral trimer with mutually perpendicular site transition dipoles, we examine interference effects in excitation transfer to a third site from symmetric and antisymmetric singly excited superposition states on the other two monomers and their quenching by electronic-vibrational coupling. In addition, we consider both electronic geometric phase development and the stabilization against internal conversion which may accompany coherent pseudo-rotational motion in the Jahn-Teller active manifold comprising two of the three singly electronically excited states.

Electronic and vibrational dynamics of an excitation-transfer trimer

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