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Surface plasmon mediated harmonically resonant effects on third harmonic generation from Au and CuS nanoparticle
Nathan J Spear1, Yueming Yan2, Joshua M Queen2
1Interdisciplinary Materials Science, Vanderbilt University, Nashville, TN 37235, USA.
Nanophotonics (Berlin, Germany)
|December 5, 2024
Summary
Dual plasmonic nanoparticle films enhance third harmonic generation (THG) through a cascaded nonlinear mechanism. Optimizing nanoparticle resonance conditions is key for efficient upconversion devices.
Area of Science:
- Materials Science
- Nanotechnology
- Nonlinear Optics
Background:
- Nonlinear materials utilize localized surface plasmonic resonance (LSPR) in nanoparticles to boost harmonic generation.
- Coupled metallic and semiconductor plasmonic nanoparticles show improved performance.
Purpose of the Study:
- Investigate dual plasmonic interactions in copper sulfide (CuS) and gold (Au) nanoparticle films.
- Analyze effects on third harmonic generation (THG).
Main Methods:
- Fabricated bilayer CuS and Au nanoparticle films.
- Studied THG under varying nanoparticle LSPR conditions relative to excitation frequency.
- Developed an analytic model for nanoparticle interactions.
Main Results:
- Detuning CuS LSPR shifted upconversion from THG to multiphoton photoluminescence (MPPL).
- Altering Au nanoparticle size eliminated enhancement by red-shifting LSPR.
- Simultaneous excitation at resonant frequencies enhanced THG via sum-frequency generation.
Conclusions:
- Enhanced THG in dually plasmonic films results from a cascaded nonlinear mechanism.
- Understanding resonance conditions is crucial for efficient THG without MPPL.
- Opens pathways for developing high-efficiency upconversion thin-film devices.

