Non-thermal emission in gap-mode plasmon photoluminescence

Robert Lemasters (), Manoj Manjare, Ryan Freeman, Feng Wang, Luka Guy Pierce, Gordon Hua, Sergei Urazhdin and Hayk Harutyunyan ()
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Robert Lemasters: Emory University
Manoj Manjare: Emory University
Ryan Freeman: Emory University
Feng Wang: Emory University
Luka Guy Pierce: Emory University
Gordon Hua: Emory University
Sergei Urazhdin: Emory University
Hayk Harutyunyan: Emory University

Nature Communications, 2024, vol. 15, issue 1, 1-8

Abstract: Abstract Photoluminescence from spatially inhomogeneous plasmonic nanostructures exhibits fascinating wavelength-dependent nonlinear behaviors due to the intraband recombination of hot electrons excited into the conduction band of the metal. The properties of the excited carrier distribution and the role of localized plasmonic modes are subjects of debate. In this work, we use plasmonic gap-mode resonators with precise nanometer-scale confinement to show that the nonlinear photoluminescence behavior can become dominated by non-thermal contributions produced by the excited carrier population that strongly deviates from the Fermi-Dirac distribution due to the confinement-induced large-momentum free carrier absorption beyond the dipole approximation. These findings open new pathways for controllable light conversion using nonequilibrium electron states at the nanoscale.

Date: 2024
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DOI: 10.1038/s41467-024-48928-4

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