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“Hot” electrons in metallic nanostructures—non-thermal carriers or heating?
Light: Science & Applications ( IF 19.4 ) Pub Date : 2019-10-02 , DOI: 10.1038/s41377-019-0199-x
Yonatan Dubi , Yonatan Sivan

Understanding the interplay between illumination and the electron distribution in metallic nanostructures is a crucial step towards developing applications such as plasmonic photocatalysis for green fuels, nanoscale photodetection and more. Elucidating this interplay is challenging, as it requires taking into account all channels of energy flow in the electronic system. Here, we develop such a theory, which is based on a coupled Boltzmann-heat equations and requires only energy conservation and basic thermodynamics, where the electron distribution, and the electron and phonon (lattice) temperatures are determined uniquely. Applying this theory to realistic illuminated nanoparticle systems, we find that the electron and phonon temperatures are similar, thus justifying the (classical) single-temperature models. We show that while the fraction of high-energy “hot” carriers compared to thermalized carriers grows substantially with illumination intensity, it remains extremely small (on the order of 10−8). Importantly, most of the absorbed illumination power goes into heating rather than generating hot carriers, thus rendering plasmonic hot carrier generation extremely inefficient. Our formulation allows for the first time a unique quantitative comparison of theory and measurements of steady-state electron distributions in metallic nanostructures.



中文翻译:

金属纳米结构中的“热”电子-非热载流子还是加热?

了解照明和金属纳米结构中电子分布之间的相互作用是迈向开发应用的关键一步,例如绿色燃料的等离激元光催化,纳米级光检测等。阐明这种相互作用是具有挑战性的,因为它需要考虑电子系统中能量流的所有通道。在这里,我们建立了这样一个理论,该理论基于耦合的玻耳兹曼-热方程,仅需要能量守恒和基本热力学,即可唯一确定电子分布以及电子和声子(晶格)温度。将这一理论应用于现实的照明纳米粒子系统,我们发现电子和声子的温度相似,从而证明了(经典)单温度模型的合理性。-8)。重要的是,大部分吸收的照明功率进入加热而不是产生热载流子,从而使等离子体热载流子的产生效率极低。我们的配方首次实现了金属纳米结构中稳态电子分布的理论和测量值的独特定量比较。

更新日期:2019-10-02
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