Winkler Jan M, Rabouw Freddy T, Rossinelli Aurelio A, Jayanti Sriharsha V, McPeak Kevin M, Kim David K, le Feber Boris, Prins Ferry, Norris David J
Optical Materials Engineering Laboratory, Department of Mechanical and Process Engineering , ETH Zurich , 8092 Zurich , Switzerland.
Nano Lett. 2019 Jan 9;19(1):108-115. doi: 10.1021/acs.nanolett.8b03422. Epub 2018 Dec 17.
Exciton polaritons are hybrid light-matter quasiparticles that can serve as coherent light sources. Motivated by applications, room-temperature realization of polaritons requires narrow, excitonic transitions with large transition dipoles. Such transitions must then be strongly coupled to an electromagnetic mode confined in a small volume. While much work has explored polaritons in organic materials, semiconductor nanocrystals present an alternative excitonic system with enhanced photostability and spectral tunability. In particular, quasi-two-dimensional nanocrystals known as nanoplatelets (NPLs) exhibit intense, spectrally narrow excitonic transitions useful for polariton formation. Here, we place CdSe NPLs on silver hole arrays to demonstrate exciton-plasmon polaritons at room temperature. Angle-resolved reflection spectra reveal Rabi splittings up to 149 meV for the polariton states. We observe bright, polarized emission arising from the lowest polariton state. Furthermore, we assess the dependence of the Rabi splitting on the hole-array pitch and the number N of NPLs. While the pitch determines the in-plane momentum for which strong coupling is observed, it does not affect the size of the splitting. The Rabi splitting first increases with NPL film thickness before eventually saturating. Instead of the commonly used [Formula: see text] dependence, we develop an analytical expression that includes the transverse confinement of the plasmon modes to describe the measured Rabi splitting as a function of NPL film thickness.
激子极化激元是一种混合的光与物质的准粒子,可作为相干光源。受应用需求的推动,室温下实现极化激元需要具有大跃迁偶极矩的窄激子跃迁。这种跃迁必须与限制在小体积内的电磁模式强耦合。虽然已有许多工作探索了有机材料中的极化激元,但半导体纳米晶体提供了另一种具有增强光稳定性和光谱可调性的激子系统。特别是,被称为纳米片(NPLs)的准二维纳米晶体表现出强烈的、光谱窄的激子跃迁,这对极化激元的形成很有用。在此,我们将CdSe纳米片放置在银孔阵列上,以展示室温下的激子 - 等离子体极化激元。角分辨反射光谱显示极化激元态的拉比分裂高达149毫电子伏特。我们观察到来自最低极化激元态的明亮、偏振发射。此外,我们评估了拉比分裂对孔阵列间距和纳米片数量N的依赖性。虽然间距决定了观察到强耦合的面内动量,但它不影响分裂的大小。拉比分裂首先随纳米片薄膜厚度增加,最终达到饱和。我们开发了一个解析表达式,该表达式包含等离子体模式的横向限制,以描述测量得到的拉比分裂随纳米片薄膜厚度的变化,而不是常用的[公式:见正文]依赖性。