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

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  • Hangyong Shan
    School of Physics, State Key Laboratory for Mesoscopic Physics, Academy for Advanced Interdisciplinary Studies, Collaborative Innovation Center of Quantum Matter, and Nano‐Optoelectronics Frontier Center of Ministry of Education Peking University Beijing 100871 China
  • Zhixin Liu
    School of Physics, State Key Laboratory for Mesoscopic Physics, Academy for Advanced Interdisciplinary Studies, Collaborative Innovation Center of Quantum Matter, and Nano‐Optoelectronics Frontier Center of Ministry of Education Peking University Beijing 100871 China
  • Xingli Wang
    CNRS International‐NTU‐Thales Research Alliance (CINTRA) Nanyang Technological University Singapore 637553 Singapore
  • Feng Lin
    School of Physics, State Key Laboratory for Mesoscopic Physics, Academy for Advanced Interdisciplinary Studies, Collaborative Innovation Center of Quantum Matter, and Nano‐Optoelectronics Frontier Center of Ministry of Education Peking University Beijing 100871 China
  • Zheng Liu
    CNRS International‐NTU‐Thales Research Alliance (CINTRA) Nanyang Technological University Singapore 637553 Singapore
  • Bo Shen
    School of Physics, State Key Laboratory for Mesoscopic Physics, Academy for Advanced Interdisciplinary Studies, Collaborative Innovation Center of Quantum Matter, and Nano‐Optoelectronics Frontier Center of Ministry of Education Peking University Beijing 100871 China
  • Jun Lou
    Department of Materials Science and NanoEngineering Rice University 6100 Main Street Houston TX 77005 USA
  • Xing Zhu
    School of Physics, State Key Laboratory for Mesoscopic Physics, Academy for Advanced Interdisciplinary Studies, Collaborative Innovation Center of Quantum Matter, and Nano‐Optoelectronics Frontier Center of Ministry of Education Peking University Beijing 100871 China
  • Pulickel M. Ajayan
    Department of Materials Science and NanoEngineering Rice University 6100 Main Street Houston TX 77005 USA
  • Zheyu Fang
    School of Physics, State Key Laboratory for Mesoscopic Physics, Academy for Advanced Interdisciplinary Studies, Collaborative Innovation Center of Quantum Matter, and Nano‐Optoelectronics Frontier Center of Ministry of Education Peking University Beijing 100871 China

Abstract

<jats:title>Abstract</jats:title><jats:p>Spontaneous 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.</jats:p>

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