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Singlet exciton fission (SEF) is initiated by ultrafast internal conversionof a singlet exciton into a correlated triplet pair (TT)1. The `reactioncoordinates' for ultrafast SEF even in archetypal systems such as pentacenethin film remain unclear with synthetic design principles broadly relying ontailoring electronic couplings to achieve new templates for efficient SEFmaterials. Spectroscopic detection of vibrational coherences in the (TT)1photoproduct has motivated theoretical investigations into a possible role ofvibronic resonance in driving SEF, akin to that reported in severalphotosynthetic proteins. However, a precise understanding of how prominentlow-frequency vibrations and their modulation of intermolecular orbitaloverlaps, equally prominent high-frequency vibrations, and order of magnitudelarger Huang-Rhys factors in SEF chromophores compared to photosyntheticpigments, collectively influence the mechanistic details of SEF remains starklylacking. Here we address this gap and identify previously unrecognized effectswhich are quite contrasting from those known in photosynthesis excitons, andvitally enhance non-adiabatic internal conversion in SEF. Our findings havedirect implications for the broad experimental interest in syntheticallytailoring molecules to promote vibronically enhanced internal conversion.

Low and High Frequency Vibrations Synergistically Enhance Singlet Exciton Fission Through Robust Vibronic Resonances