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We show that the dynamics of (vertical) Franck-Condon excitations in theregime where Holstein-coupled vibrational modes mix strongly with electronicdegrees of freedom sharply contrasts with the known self-localized behavior ofvibrationally relaxed excitations. Instead, the strongly-coupled modes arefound to periodically induce resonances between interacting electronic sites,during which effective excitation transfer occurs, allowing Franck-Condonexcitations to attain substantial mean square displacements under conditionswhere relaxed excitations are essentially trapped to a single site. Indemonstrating this behavior, we employ a multi-set matrix product stateformalism. We find this numerically exact technique to be a remarkablyefficient approach to the notoriously difficult problem posed by the Holsteinmodel in the regime where the electronic coupling, the vibrational quantum, andthe vibrational reorganization energy are comparable in magnitude.

Multi-set matrix product state calculations reveal mobile Franck-Condon excitations under strong Holstein-type coupling