Angle-Independent Polariton Emission Lifetime Shown by Perylene Hybridized to the Vacuum Field Inside a Fabry-Pérot Cavity.
Angle-Independent Polariton Emission Lifetime Shown by Perylene Hybridized to the Vacuum Field Inside a Fabry-Pérot Cavity.
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DOI：
10.1021/acs.jpcc.8b07283
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发表时间：
2018-11-01
期刊：
影响因子：
--
通讯作者：
Börjesson K
中科院分区：
文献类型：
--
作者：
Mony J;Hertzog M;Kushwaha K;Börjesson K
光-物质混合态在光学结构中的形成，表现为耦合系统本征能量的拉比分裂，是量子光学中的关键效应之一。混合态（激子极化激元）具有独特的化学和物理性质，可以被视为光和物质的线性组合。激子极化激元的光学性质本质上是色散的，这是从光子对极化激元的贡献继承的性质。另一方面，有机分子体系中的极化激元寿命最近引起了很大的争论。光子对极化激元的贡献表明其寿命在飞秒时间尺度上，比实验观察到的要短得多。在这里，我们增加了光物质状态的见解表明，极化激元发射寿命是非色散的。通过将二萘嵌苯衍生物结合到法布里-佩罗腔中，将其与真空场强耦合。从腔中的极化激元发射被证明是色散的，但发射寿命是非色散的和裸激子的时间尺度上。激子库模型使结果合理化，为目前使用的理论提供了实验证据，从而提高了我们对分子中强耦合现象的理解。
The formation of hybrid light–matter states in optical structures, manifested as a Rabi splitting of the eigenenergies of a coupled system, is one of the key effects in quantum optics. The hybrid states (exciton polaritons) have unique chemical and physical properties and can be viewed as a linear combination of light and matter. The optical properties of the exciton polaritons are dispersive by nature, a property inherited from the photonic contribution to the polariton. On the other hand, the polariton lifetime in organic molecular systems has recently been highly debated. The photonic contribution to the polariton would suggest a lifetime on the femtosecond time scale, much shorter than experimentally observed. Here, we increase the insights of light–mater states by showing that the polariton emission lifetime is nondispersive. A perylene derivative was strongly coupled to the vacuum field by incorporating the molecule into a Fabry–Pérot cavity. The polariton emission from the cavity was shown to be dispersive, but the emission lifetime was nondispersive and on the time scale of the bare exciton. The results were rationalized by the exciton reservoir model, giving experimental evidence to currently used theories, thus improving our understanding of strong coupling phenomena in molecules.
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影响因子：
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作者：
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