The photochemistry of a molecular ensemble coupled to a resonance cavity and triggered by a femtosecond laser pulse is investigated from a real-time, quantum dynamics perspective with the multi-configuration time-dependent Hartree method. Coherent excitation of a superposition of electronic states in the ensemble leads to superradiant energy transfer to the cavity characterized by quadratic scaling with the number of molecules. Electronic decoherence associated with loss of nuclear wave packet overlap among those states destroys superradiant energy transfer, returning to a linear regime. For equal pump laser conditions, the photoexcitation probability per molecule decreases with increase of the number of molecules inside the cavity. This is caused by a loss of resonance condition of the laser with the bright electronic-photonic states of the coupled cavity-ensemble system. Increase of the laser bandwidth restores the energy transferred per molecule and the trigger probability remains independent of the number of molecules in the cavity.

从实时，量子动力学的角度，使用多组态时变哈特里方法，研究了耦合到共振腔并由飞秒激光脉冲触发的分子团的光化学。集合体中电子态叠加的相干激发导致超辐射能量转移腔的特征是随着分子数量的二次缩放。与这些状态之间的核波包重叠丢失相关的电子退相干破坏了超辐射能的传递，回到了线性状态。对于相等的泵浦激光条件，每个分子的光激发概率随着腔体内分子数量的增加而降低。这是由于耦合腔腔集成系统的明亮电子光子状态下的激光谐振条件的损失引起的。激光带宽的增加恢复了每个分子传递的能量，并且触发概率与腔中分子的数量无关。