Temporal Dynamics of Localized Exciton–Polaritons in Composite Organic–Plasmonic Metasurfaces,Nano Letters

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Temporal Dynamics of Localized Exciton–Polaritons in Composite Organic–Plasmonic Metasurfaces
Nano Letters ( IF 9.6 ) Pub Date : 2017-11-02 00:00:00 , DOI: 10.1021/acs.nanolett.7b03751
Elad Eizner ₁ , Katherine Akulov ₁ , Tal Schwartz ₁ , Tal Ellenbogen ₁

Affiliation

We use femtosecond transient absorption spectroscopy to study the temporal dynamics of strongly coupled exciton–plasmon polaritons in metasurfaces of aluminum nanoantennas coated with J-aggregate molecules. Compared with the thermal nonlinearities of aluminum nanoantennas, the exciton–plasmon hybridization introduces strong ultrafast nonlinearities in the composite metasurfaces. Within femtoseconds after the pump excitation, the plasmonic resonance is broadened and shifted, showcasing its high sensitivity to excited-state modification of the molecular surroundings. In addition, we observe temporal oscillations due to the deep subangstrom acoustic breathing modes of the nanoantennas in both bare and hybrid metasurfaces. Finally, unlike the dynamics of hybrid states in optical microcavities, here, ground-state bleaching is observed with a significantly longer relaxation time at the upper polariton band.

中文翻译：

复合有机-肺超表面中局部激子-波兰蛋白的时间动态

我们使用飞秒瞬态吸收光谱法研究了涂有J聚集分子的铝纳米天线的超表面中强耦合激子-等离激元极化子的时间动态。与铝纳米天线的热非线性相比，激子-等离子体激元杂交在复合超表面中引入了强大的超快非线性。在泵浦激发后的飞秒内，等离子体共振变宽并发生位移，这表明其对分子周围环境的激发态修饰具有很高的敏感性。另外，我们观察到由于在裸表面和混合表面中纳米天线的深亚埃级声呼吸模式而引起的时间振荡。最后，与光学微腔中混合态的动力学不同，在这里，

更新日期：2017-11-02

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