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Plasmon-Amplified Third Harmonic Generation in Metal/Dielectric Resonators

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Enhancing ultrafast nonlinear processes at a nanometer scale has the potential of creating novel nano-sources of energetic photons or particles useful for many applications, especially for embedded diagnostics. In this work, we investigate the plasmonic amplification of the third harmonic generation (THG) from a metal-dielectric-metal (MDM) nano-resonator in the near-terawatt intensity regime. In our geometry, the Fabry-Pérot plasmonic resonator reaches a high local enhancement of the laser electric field over a large volume of a SiO2 dielectric film. The THG signal is amplified by more than one order of magnitude, with a higher efficiency compared to previous plasmonic geometries. The polarization dependence with respect to the fundamental laser allows an ON/OFF switch of the THG enhancement in the nanostructures which is a strong signature of the plasmonic origin of the THG amplification. Furthermore, the dispersion scan shows that the third harmonic spectrum is strongly redshifted with respect to the peak of its linear extinction spectrum. Using the nonlinear anharmonic model, we confirm that the third harmonic behavior dominantly arises from the silica layer.

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Data Availability

The datasets generated during and/or analyzed during the current study are available from the corresponding author on reasonable request

Code Availability

The codes used during the current study are available from the corresponding author on reasonable request.


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We received financial support from the European Union through the Future and Emerging Technologies (FET) Open H2020: PETACom (grant 829153), OPTOLOGIC (grant 899794). Support from the DGA RAPID grant “SWIM,” from the Centre National de Compétences en Nanosciences (C’NANO) research program through the NanoscopiX grant; the LABoratoire d’EXcelence Physique Atoms Lumière Matière—LABEX PALM (ANR-10-LABX-0039-PALM), through the grants “Plasmon-X” and “STAMPS” and, finally, the Action de Soutien à la Technologie et à la Recherche en Essonne (ASTRE) program through the “NanoLight” grant are also acknowledged. Support from the French National Research Agency through the PACHA grant (ANR-17-CE30-0008–01). Financial support by the German Research Foundation, grant KO 3798/4–1 and from Germany’s Excellence Strategy EXC-2123 and Germany’s Excellence Strategy within the Cluster of Excellence PhoenixD (EXC 2122, Project ID 390833453), Lower Saxony through “Quanten und Nanometrologie” (QUANOMET, Project Nanophotonik).

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All the authors contributed to the study conception and design. Conceptualization of the experiment was done by Hamed Merdji and Milutin Kovacev and Rana Nicolas. Material preparation, data collection, and analysis were performed by Rana Nicolas, Liping Shi. The analysis of the results was done by all authors. First draft of the manuscript was written by Rana Nicolas, and all the authors commented on previous versions of the manuscript. All the authors read and approved the final manuscript.

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Correspondence to Rana Nicolas.

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Nicolas, R., Shi, L., Chanteau, B. et al. Plasmon-Amplified Third Harmonic Generation in Metal/Dielectric Resonators. Plasmonics 16, 1883–1889 (2021).

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