Determining plasmonic hot-carrier energy distributions via single-molecule transport measurements
Determining plasmonic hot-carrier energy distributions via single-molecule transport measurements
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DOI：
10.1126/science.abb3457
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发表时间：
2020-07-24
期刊：
影响因子：
56.9
通讯作者：
Meyhofer, Edgar
中科院分区：
文献类型：
--
作者：
Reddy, Harsha;Wang, Kun;Meyhofer, Edgar
通过等离子体衰变产生的等离子体纳米结构中的热载流子在诸如MEMS和规避带隙限制的光电探测器的应用中发挥关键作用。然而，到目前为止，在纳米结构中的热载流子的稳态能量分布的直接实验量化一直缺乏。我们目前的运输测量单分子结，通过捕获适当选择的单分子之间的支持表面等离子体激元和扫描探针针尖，可以提供定量的等离子体激元热载流子分布的金膜。我们的研究结果表明，朗道阻尼是纳米尺度系统中热载流子产生的主要物理机制。在这项工作中开发的技术将使纳米光子和等离子体激元器件中的等离子体激元热载流子分布的量化。
Hot carriers in plasmonic nanostructures, generated via plasmon decay, play key roles in applications such as photocatalysis and in photodetectors that circumvent bandgap limitations. However, direct experimental quantification of steady-state energy distributions of hot carriers in nanostructures has so far been lacking. We present transport measurements from single-molecule junctions, created by trapping suitably chosen single molecules between an ultrathin gold film supporting surface plasmon polaritons and a scanning probe tip, that can provide quantification of plasmonic hot-carrier distributions. Our results show that Landau damping is the dominant physical mechanism of hot-carrier generation in nanoscale systems with strong confinement. The technique developed in this work will enable quantification of plasmonic hot-carrier distributions in nanophotonic and plasmonic devices.