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

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

doi:10.1126/science.abb3457

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

Journal Article · Thu Jun 04 00:00:00 EDT 2020 · Science

DOI:https://doi.org/10.1126/science.abb3457· OSTI ID:1781912

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School of Electrical and Computer Engineering, Purdue University, West Lafayette, IN 47907, USA.
Department of Mechanical Engineering, University of Michigan, Ann Arbor, MI 48109, USA.
School of Electrical and Computer Engineering, Purdue University, West Lafayette, IN 47907, USA., Center for Science of Information, Purdue University, West Lafayette, IN 47907, USA.
Department of Chemistry, University of Liverpool, Liverpool L69 7ZD, UK.
Department of Mechanical Engineering, University of Michigan, Ann Arbor, MI 48109, USA., Department of Materials Science and Engineering, University of Michigan, Ann Arbor, MI 48109, USA.

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.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0004871

OSTI ID:: 1781912

Alternate ID(s):: OSTI ID: 1801606

Journal Information:: Science, Journal Name: Science Journal Issue: 6502 Vol. 369; ISSN 0036-8075

Publisher:: American Association for the Advancement of Science (AAAS)Copyright Statement

Country of Publication:: United States

Language:: English

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