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We recently proposed effective normal modes for excitonically coupledaggregates which exactly transform the energy transfer Hamiltonian into a sumof one-dimensional Hamiltonians along the effective normal modes. Identifyingphysically meaningful vibrational motions which maximally promote vibronicmixing suggested an interesting possibility of leveragingvibrational-electronic resonance for mediating selective energy transfer. Herewe expand on the effective mode approach elucidating its iterative nature forsuccessively larger aggregates, and extend the idea of mediated energy transferto larger aggregates. We show that energy transfer between electronicallyuncoupled but vibronically resonant donor-acceptor sites does not depend on theintermediate site energy or the number of intermediate sites. The intermediatesites simply mediate electronic coupling such that vibronic coupling alongspecific promoter modes leads to direct donor-acceptor energy transferbypassing any intermediate uphill energy transfer steps. We show that interplaybetween the electronic Hamiltonian and the effective mode transformationpartitions the linear vibronic coupling along specific promoter modes todictate the selectivity of mediated energy transfer, with a vital role ofinterference between vibronic couplings and multi-particle basis states. Ourresults suggest a general design principle for enhancing energy transferthrough synergistic effects of vibronic resonance and weak mediated electroniccoupling, where both effects individually do not promote efficient energytransfer. The effective mode approach proposed here paves a facile routetowards four-wavemixing spectroscopy simulations of larger aggregates withoutseverely approximating resonant vibronic coupling.

Vibronic Resonance Along Effective Modes Mediates Selective Energy Transfer in Excitonically Coupled Aggregates