Determining plasmonic hot-carrier energy distributions via single-molecule transport measurements

Reddy, Harsha, Wang, Kun, Kudyshev, Zhaxylyk, Zhu, Linxiao, Yan, Shen, Vezzoli, Andrea ORCID: 0000-0002-8059-0113, Higgins, Simon J ORCID: 0000-0003-3518-9061, Gavini, Vikram, Boltasseva, Alexandra, Reddy, Pramod
et al (show 2 more authors) (2020) Determining plasmonic hot-carrier energy distributions via single-molecule transport measurements. SCIENCE, 369 (6502). 423 - 426.

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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.

Item Type: Article
Depositing User: Symplectic Admin
Date Deposited: 07 Sep 2020 09:40
Last Modified: 01 May 2021 19:10
DOI: 10.1126/science.abb3457
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