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通过与法布里-珀罗腔内真空场杂交的苝显示的与角度无关的极化激元发射寿命。

Angle-Independent Polariton Emission Lifetime Shown by Perylene Hybridized to the Vacuum Field Inside a Fabry-Pérot Cavity.

作者信息

Mony Jürgen, Hertzog Manuel, Kushwaha Khushbu, Börjesson Karl

机构信息

Department of Chemistry and Molecular Biology, University of Gothenburg, Kemigården 4, Gothenburg 41296, Sweden.

出版信息

J Phys Chem C Nanomater Interfaces. 2018 Nov 1;122(43):24917-24923. doi: 10.1021/acs.jpcc.8b07283. Epub 2018 Oct 4.

Abstract

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.

摘要

光学结构中混合光-物质态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,可视为光与物质的线性组合。激子极化激元的光学性质本质上是色散的,这一性质继承自极化激元中的光子成分。另一方面,有机分子系统中极化激元的寿命最近备受争议。极化激元中的光子成分表明其寿命在飞秒时间尺度,远短于实验观测结果。在此,我们通过表明极化激元发射寿命是非色散的,增进了对光-物质态的理解。通过将苝衍生物分子纳入法布里-珀罗腔,使其与真空场发生强耦合。腔中极化激元的发射表现为色散的,但其发射寿命是非色散的,且处于裸激子的时间尺度。激子库模型对这些结果进行了合理解释,为当前使用的理论提供了实验证据,从而增进了我们对分子中强耦合现象的理解。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9ae5/6234983/5bf00f3a4de6/jp-2018-07283f_0001.jpg

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