Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104, USA.
Nano Lett. 2013 Jun 12;13(6):2857-63. doi: 10.1021/nl4012003. Epub 2013 May 29.
The influence of particle shape on plasmonic response and local electric field strength is well-documented in metallic nanoparticles. Morphologies such as rods, plates, and octahedra are readily synthesized and exhibit drastically different extinction spectra than spherical particles. Despite this fact, the influence of composition and shape on the optical properties of plasmonic semiconductor nanocrystals, in which free electrons result from heavy doping, has not been well-studied. Here, we report the first observation of plasmonic resonance in indium-doped cadmium oxide (ICO) nanocrystals, which exhibit the highest quality factors reported for semiconductor nanocrystals. Furthermore, we are able to independently control the shape and free electron concentration in ICO nanocrystals, allowing for the influence of shape on the optical response of a plasmonic semiconductor to be conclusively demonstrated. The highly uniform particles may be self-assembled into ordered single component and binary nanocrystal superlattices, and in thin films, exhibit negative permittivity in the near infrared (NIR) region, validating their use as a new class of tunable low-loss plasmonic building blocks for 3-D optical metamaterials.
在金属纳米粒子中,颗粒形状对等离子体响应和局域电场强度的影响已有大量文献记载。棒状、板状和八面体等形态很容易合成,并且表现出与球形粒子截然不同的消光谱。尽管如此,对于由重掺杂产生自由电子的等离子体半导体纳米晶体的组成和形状对光学性质的影响,还没有得到很好的研究。在这里,我们首次观察到掺铟氧化镉(ICO)纳米晶体中的等离子体共振,其品质因数是报道的半导体纳米晶体中最高的。此外,我们能够独立控制 ICO 纳米晶体的形状和自由电子浓度,从而可以明确证明形状对等离子体半导体光学响应的影响。这些高度均匀的颗粒可以自组装成有序的单相和二元纳米晶体超晶格,在薄膜中,在近红外(NIR)区域表现出负介电常数,验证了它们作为一类新的可调谐低损耗等离子体构建块用于 3D 光学超材料的用途。