定向电子束辐照对纳米粒子等离子体响应的雕刻
Sculpting the plasmonic responses of nanoparticles by directed electron beam irradiation
摘要：
功能纳米结构中物质的空间限制将这些系统推向了纳米科学的最前沿，既作为奇异物理和量子现象的游乐场，又在包括等离子体、光电子和传感在内的多种应用中。与此同时，单色电子能量损失谱（EELS）的出现使得能够探索单个纳米颗粒内的局部纳米等离子体功能和纳米颗粒组装体的集体响应，从而深入了解相关机制。然而，等离子体纳米结构的现代合成工艺通常限于可访问的几何形状和材料的类型，并且即使如此，也限于数十nm量级的空间精度，从而排除了对结构-性质关系的关键方面的直接探索。在这里，我们使用扫描透射电子显微镜（STEM）的原子大小探针来执行纳米颗粒配置的精确雕刻和设计。此外，使用低损耗（EELS），我们提供了动态分析的等离子体激元响应的演变过程中的雕刻过程。我们表明，在纳米粒子的自组装系统中，单个纳米粒子可以选择性地去除，重塑或以纳米级分辨率任意图案化，有效地修改空间和能量域中的等离子体响应。这一过程大大增加了设计的可能性，并为任意结构的开发提供了机会，这最终是纳米光子设计的关键。纳米雕刻又给电子显微镜带来了另一种能力。
英文摘要：
Spatial confinement of matter in functional nanostructures has propelled these systems to the forefront of nanoscience, both as a playground for exotic physics and quantum phenomena and in multiple applications including plasmonics, optoelectronics, and sensing. In parallel, the emergence of monochromated electron energy loss spectroscopy (EELS) has enabled exploration of local nanoplasmonic functionalities within single nanoparticles and the collective response of nanoparticle assemblies, providing deep insight into the associated mechanisms. However, modern synthesis processes for plasmonic nanostructures are often limited in the types of accessible geometry and materials, and even then, limited to spatial precisions on the order of tens of nm, precluding the direct exploration of critical aspects of the structure-property relationships. Here, we use the atomic-sized probe of the scanning transmission electron microscope (STEM) to perform precise sculpting and design of nanoparticle configurations. Furthermore, using low-loss (EELS), we provide dynamic analyses of evolution of the plasmonic response during the sculpting process. We show that within self-assembled systems of nanoparticles, individual nanoparticles can be selectively removed, reshaped, or arbitrarily patterned with nanometer-level resolution, effectively modifying the plasmonic response in both space and energy domains. This process significantly increases the scope for design possibilities and presents opportunities for arbitrary structure development, which are ultimately key for nanophotonic design. Nanosculpting introduces yet another capability to the electron microscope.
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