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The photochemistry of a molecular ensemble coupled to a resonance cavity andtriggered by a femtosecond laser pulse is investigated from a real-time,quantum dynamics perspective with the multi-configuration time-dependentHartree method. Coherent excitation of a superposition of electronic states inthe ensemble leads to superradiant energy transfer to the cavity characterizedby quadratic scaling with the number of molecules. Electronic decoherenceassociated with loss of nuclear wave packet overlap among those states destroyssuperradiant energy transfer, returning to a linear regime. For equal pumplaser conditions, the photoexcitation probability per molecule decreases withincrease of the number of molecules inside the cavity. This is caused by a lossof resonance condition of the laser with the bright electronic-photonic statesof the coupled cavity-ensemble system. Increase of the laser bandwidth restoresthe energy transferred per molecule and the trigger probability remainsindependent of the number of molecules in the cavity.

Coherent dynamics in cavity femtochemistry: application of the multi-configuration time-dependent Hartree method