NanoEngineering Department, University of California, San Diego , La Jolla, California 92093-0448, United States.
Nano Lett. 2014 May 14;14(5):2372-80. doi: 10.1021/nl404777h. Epub 2014 Apr 22.
Semiconductor nanocrystals are key materials for achieving localized surface plasmon resonance (LSPR) excitation in the extended spectral ranges beyond visible light, which are critical wavelengths for chemical sensing, infrared detection, and telecommunications. Unlike metal nanoparticles which are already widely exploited in plasmonics, little is known about the near-field behavior of semiconductor nanocrystals. Near-field interactions are expected to vary greatly with nanocrystal carrier density and mobility, in addition to properties such as nanocrystal size, shape, and composition. Here we demonstrate near-field coupling between anisotropic disk-shaped nanocrystals composed of Cu2-xS, a degenerately doped semiconductor whose electronic properties can be modulated by Cu content. Assembling colloidal nanocrystals into mono- and multilayer films generates dipole-dipole LSPR coupling between neighboring nanodisks. We investigate nanodisks of varying crystal phases (Cu1.96S, Cu7.2S4, and CuS) and find that nanodisk orientation produces a dramatic change in the magnitude and polarization direction of the localized field generated by LSPR excitation. This study demonstrates the potential of semiconductor nanocrystals for the realization of low-cost, active, and tunable building blocks for infrared plasmonics and for the investigation of light-matter interactions at the nanoscale.
半导体纳米晶体是实现局部表面等离子体共振(LSPR)激发的关键材料,激发范围扩展至可见光之外的光谱区域,这些区域对于化学传感、红外探测和电信至关重要。与已经广泛应用于等离子体学的金属纳米粒子不同,对于半导体纳米晶体的近场行为知之甚少。除了纳米晶体的尺寸、形状和组成等性质外,近场相互作用预计会随着纳米晶体的载流子密度和迁移率而发生很大变化。在这里,我们展示了由 Cu2-xS 组成的各向异性盘状纳米晶体之间的近场耦合,Cu2-xS 是一种简并掺杂的半导体,其电子性质可以通过 Cu 含量进行调制。将胶体纳米晶体组装成单分子层和多层薄膜会在相邻纳米盘之间产生偶极-偶极 LSPR 耦合。我们研究了具有不同晶体相(Cu1.96S、Cu7.2S4 和 CuS)的纳米盘,并发现纳米盘的取向会导致由 LSPR 激发产生的局域场的幅度和偏振方向发生显著变化。这项研究展示了半导体纳米晶体在实现低成本、有源和可调谐的红外等离子体学构建块以及在纳米尺度上研究光物质相互作用方面的潜力。