TY - JOUR
T1 - Determining plasmonic hot-carrier energy distributions via single-molecule transport measurements
AU - Reddy, Harsha
AU - Wang, Kun
AU - Kudyshev, Zhaxylyk
AU - Zhu, Linxiao
AU - Yan, Shen
AU - Vezzoli, Andrea
AU - Higgins, Simon J.
AU - Gavini, Vikram
AU - Boltasseva, Alexandra
AU - Reddy, Pramod
AU - Shalaev, Vladimir M.
AU - Meyhofer, Edgar
N1 - Funding Information:
The work was supported by a grant from the Army Research Office [grant W911NF-19-1-0279 to P.R., V.M.S., and E.M. (design of plasmonic structures and modeling)]. P.R. and E.M. acknowledge support from the Department of Energy [DOE-BES award DE-SC0004871 (scanning probe measurements and analysis)], the U.S. Office of Naval Research [ONR award N00014-16-1-2672 (synthesis of H1)], and the U.S. National Science Foundation, award 1803983). V.G., P.R., and E.M. thank the Department of Mechanical Engineering at the University of Michigan for support via a RIP-ME grant (DFT calculations). A.B. and V.M.S. acknowledge support from the Air Force Office of Scientific Research grants FA9550-17-1-0243 and FA9550-20- 1-0124 (realization of ultrathin gold films and surface plasmon structures). V.G. acknowledges the support of the Army Research Office for a DURIP award (grant W911NF1810242), which provided the computational resources for the DFT calculations. A.V. and S.J.H. acknowledge support from the EPSRC (grant EP/M029522/1).
Publisher Copyright:
© 2020 American Association for the Advancement of Science. All rights reserved.
PY - 2020/7/24
Y1 - 2020/7/24
N2 - 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.
AB - 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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U2 - 10.1126/science.abb3457
DO - 10.1126/science.abb3457
M3 - Article
C2 - 32499398
AN - SCOPUS:85088608491
SN - 0036-8075
VL - 369
SP - 423
EP - 426
JO - Science
JF - Science
IS - 6502
ER -