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Determining Plasmonic Hot-carrier Energy Distributions Via Single-molecule Transport Measurements

Harsha Reddy, Kun Wang, Zhaxylyk Kudyshev, Linxiao Zhu, Shen Yan, Andrea Vezzoli, Simon J. Higgins, Vikram Gavini, Alexandra Boltasseva, Pramod Reddy, Vladimir M. Shalaev, Edgar Meyhofer

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Hot-carriers in plasmonic nanostructures, generated via plasmon decay, play key roles in applications like photocatalysis and in photodetectors that circumvent band-gap 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 ultra-thin 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.