Spontaneous Emission of Plasmon‐Exciton Polaritons Revealed by Ultrafast Nonradiative Decays

Abstract

AbstractSpontaneous emission can be altered by external electromagnetic environment with the bridge of local density of optical states. Microcavities have been widely integrated to accelerate the irreversible spontaneous decay, known as the Purcell effect. However, the Purcell effect breaks down in the strong coupling regime, where the light‐matter interaction is not a perturbation to Fermi's golden rule. Here, it is found that the emission intensity of plasmon–exciton polaritons is asymmetrically dependent on the spectral detuning, confirming the collapse of Purcell effect in strongly coupled systems. Ultrafast nonradiative decays of polaritons play a significant role in revealing the polariton emission intensity. The nonradiative effect is not affected by the coherent energy exchange since final states of nonradiative decays are optically dark and decoupled from Rabi oscillations. Moreover, the nonradiative effect is still valid under intermediate coupling and agrees with the Purcell effect, which suggests its universality at a variety of coupling regimes. This study opens up a successful approach to investigate spontaneous emission in cavity quantum electrodynamics, which is insightful to photonic and opto‐electronic applications based on exciton‐polaritons.