超快无辐射衰变揭示了等离子体激子极化子的自发发射。,Laser & Photonics Reviews

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超快无辐射衰变揭示了等离子体激子极化子的自发发射。
Laser & Photonics Reviews ( IF 9.8 ) Pub Date : 2020-09-15 , DOI: 10.1002/lpor.202000233
Hangyong Shan ₁ , Zhixin Liu ₁ , Xingli Wang ₂ , Feng Lin ₁ , Zheng Liu ₂ , Bo Shen ₁ , Jun Lou ₃ , Xing Zhu ₁ , Pulickel M. Ajayan ₃ , Zheyu Fang ₁

Affiliation

自发发射可以通过外部电磁环境和光学状态局部密度的桥梁来改变。微腔已被广泛集成以加速不可逆的自发衰减，这被称为珀塞尔效应。但是，珀塞尔效应在强耦合机制下破裂，在这种耦合机制下，光与物质的相互作用不会干扰费米的黄金定律。在这里，我们发现等离子激子极化子的发射强度不对称地取决于光谱失谐，这证实了强耦合系统中赛尔效应的崩溃。极化子的超快非辐射衰减在揭示极化子发射强度方面起着重要作用。非辐射效应不受相干能量交换的影响，因为非辐射衰变的最终状态在光学上是暗的，并且与拉比振荡不相关。而且，非辐射效应在中间偶联作用下仍然有效，并且与珀塞尔效应一致，这表明其在多种偶联机制下具有普遍性。这项研究为研究腔量子电动力学中的自发发射开辟了一条成功的途径，这对于基于激子极化子的光子和光电应用具有深刻的见解。

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

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.

更新日期：2020-09-15

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