Data from: Hot Carrier Extraction with Plasmonic Broadband Absorbers

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Hot charge carrier extraction from metallic nanostructures is a very promising approach for applications in photocatalysis, photovoltaics, and photodetection. One limitation is that many metallic nanostructures support a single plasmon resonance thus restricting the light-to-charge-carrier activity to a spectral band. Here we demonstrate that a monolayer of plasmonic nanoparticles can be assembled on a multistack layered configuration to achieve broadband, near-unit light absorption, which is spatially localized on the nanoparticle layer. We show that this enhanced light absorbance leads to 40-fold increases in the photon-to-electron conversion efficiency by the plasmonic nanostructures. We developed a model that successfully captures the essential physics of the plasmonic hot electron charge generation and separation in these structures. This model also allowed us to establish that efficient hot carrier extraction is limited to spectral regions where (i) the photons have energies higher than the Schottky junctions and (ii) the absorption of light is localized on the metal nanoparticles.

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从金属纳米结构中提取热载流子，是光催化、光伏及光电探测领域极具应用前景的技术路径。但该技术存在一项局限：多数金属纳米结构仅支持单一等离子体共振（plasmon resonance）模式，导致光-载流子转化活性被限制在单一光谱波段内。本研究证明，可将等离子体纳米颗粒单层组装于多层堆叠结构中，从而实现宽带、近单位光吸收，且该吸收过程空间局域于纳米颗粒层。研究表明，这种增强的光吸收能力可使等离子体纳米结构的光子-电子转化效率提升40倍。本研究构建了一个模型，可精准捕捉这类结构中等离子体热电子的电荷产生与分离过程的核心物理机制。借助该模型，我们还明确了高效热载流子提取仅适用于两类光谱区域：(1) 光子能量高于肖特基结（Schottky junction）；(2) 光吸收过程局域于金属纳米颗粒之上。