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Plasmon-Amplified Third Harmonic Generation in Metal/Dielectric Resonators

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Abstract

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.

References

  1. Franken PA, Hill AE, Peters CW, Weinreich G (1961) Generation of optical harmonics. Phys Rev Lett 7(4):118–119. https://doi.org/10.1103/PhysRevLett.7.118

    Article  Google Scholar 

  2. Shi L et al (2019) Generating ultrabroadband deep-UV radiation and sub-10 nm Gap by hybrid-morphology gold antennas. Nano Lett 19(7):4779–4786. https://doi.org/10.1021/acs.nanolett.9b02100

    Article  CAS  PubMed  Google Scholar 

  3. Stockman MI et al (2018) Roadmap on plasmonics. J Opt 20(4):043001. https://doi.org/10.1088/2040-8986/aaa114

    Article  CAS  Google Scholar 

  4. Panoiu NC, Sha WEI, Lei DY, Li G-C (2018) Nonlinear optics in plasmonic nanostructures. J Opt 20(8):083001. https://doi.org/10.1088/2040-8986/aac8ed

    Article  CAS  Google Scholar 

  5. Celebrano M et al (2015) Mode matching in multiresonant plasmonic nanoantennas for enhanced second harmonic generation. Nat Nanotechnol 10(5):412–417. https://doi.org/10.1038/nnano.2015.69

    Article  CAS  PubMed  Google Scholar 

  6. Hentschel M, Utikal T, Giessen H, Lippitz M (2012) Quantitative modeling of the third harmonic emission spectrum of plasmonic nanoantennas. Nano Lett 12(7):3778–3782. https://doi.org/10.1021/nl301686x

    Article  CAS  PubMed  Google Scholar 

  7. Metzger B, Hentschel M, Lippitz M, Giessen H (2012) Third-harmonic spectroscopy and modeling of the nonlinear response of plasmonic nanoantennas. Opt Lett 37(22):4741–4743. https://doi.org/10.1364/OL.37.004741

    Article  CAS  PubMed  Google Scholar 

  8. Lippitz M, van Dijk MA, Orrit M (2005) Third-harmonic generation from single gold nanoparticles. Nano Lett 5(4):799–802. https://doi.org/10.1021/nl0502571

    Article  CAS  PubMed  Google Scholar 

  9. Shi L et al (2017) Self-optimization of plasmonicnanoantennas in strong femtosecond fields. Optica 4(9):1038–1043. https://doi.org/10.1364/OPTICA.4.001038

    Article  CAS  Google Scholar 

  10. Chandran A, Barnard ES, White JS, Brongersma ML (2012) Metal-dielectric-metal surface plasmon-polariton resonators. Phys Rev B 85(8):085416. https://doi.org/10.1103/PhysRevB.85.085416

    Article  Google Scholar 

  11. Shibanuma T, Grinblat G, Albella P, Maier SA (2017) Efficient third harmonic generation from metal–dielectric hybrid nanoantennas. Nano Lett. https://doi.org/10.1021/acs.nanolett.7b00462

    Article  PubMed  Google Scholar 

  12. Shi L et al (2018) Resonant-plasmon-assisted subwavelength ablation by a femtosecond oscillator. Phys Rev Appl 9(2):024001. https://doi.org/10.1103/PhysRevApplied.9.024001

    Article  CAS  Google Scholar 

  13. de Ceglia D, Vincenti MA, Akozbek N, Bloemer MJ, Scalora M (2017) Nested plasmonic resonances: extraordinary enhancement of linear and nonlinear interactions. Opt Express 25(4):3980–3990. https://doi.org/10.1364/OE.25.003980

    Article  PubMed  Google Scholar 

  14. Javůrek D, Peřina J (2019) Analytical model of surface second-harmonic generation. Sci Rep 9(1):1–12. https://doi.org/10.1038/s41598-019-39260-9

    Article  CAS  Google Scholar 

  15. Huang JP, Yu KW (2007) New nonlinear optical materials: theoretical research. Nova Publishers.

  16. Han S et al (2016) High-harmonic generation by field enhanced femtosecond pulses in metal-sapphire nanostructure. Nat Commun 7:13105. https://doi.org/10.1038/ncomms13105

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  17. Yu H, Peng Y, Yang Y, Li ZY (2019) Plasmon-enhanced light–matter interactions and applications. Npj Comput Mater 5(1):1–14. https://doi.org/10.1038/s41524-019-0184-1

    Article  Google Scholar 

  18. Yu C, Jiang S, Lu R (2019) High order harmonic generation in solids: a review on recent numerical methods. Adv Phys X 4(1):1562982. https://doi.org/10.1080/23746149.2018.1562982

    Article  CAS  Google Scholar 

  19. Vampa G et al (2017) Plasmon-enhanced high-harmonic generation from silicon. Nat Phys 13(7):7. https://doi.org/10.1038/nphys4087

  20. Renger J, Quidant R, Novotny L (2011) Enhanced nonlinear response from metal surfaces. Opt Express 19(3):1777–1785. https://doi.org/10.1364/OE.19.001777

    Article  CAS  PubMed  Google Scholar 

  21. Khurgin JB (2015) How to deal with the loss in plasmonics and metamaterials. Nat Nanotechnol 10:2–6. https://doi.org/10.1038/nnano.2014.310

    Article  CAS  PubMed  Google Scholar 

  22. Kauranen M, Zayats AV (2012) Nonlinear plasmonics. Nat Photonics 6(11):737–748. https://doi.org/10.1038/nphoton.2012.244

    Article  CAS  Google Scholar 

  23. Butet J, Brevet P-F, Martin OJF (2015) Optical second harmonic generation in plasmonic nanostructures: from fundamental principles to advanced applications. ACS Nano 9(11):10545–10562. https://doi.org/10.1021/acsnano.5b04373

    Article  CAS  PubMed  Google Scholar 

  24. Shaaran T et al (2017) Nano-plasmonic near field phase matching of attosecond pulses. Sci Rep 7. https://doi.org/10.1038/s41598-017-06491-7

  25. Metzger B et al (2014) Doubling the efficiency of third harmonic generation by positioning ITO nanocrystals into the hot-spot of plasmonic gap-antennas. Nano Lett 14(5):2867–2872. https://doi.org/10.1021/nl500913t

    Article  CAS  PubMed  Google Scholar 

  26. Plasmonics: Fundamentals and Applications | Stefan Alexander Maier | Springer

  27. Accanto N, Piatkowski L, Renger J, van Hulst NF (2014) Capturing the optical phase response of nanoantennas by coherent second-harmonic microscopy. Nano Lett 14(7):4078–4082. https://doi.org/10.1021/nl501588r

    Article  CAS  PubMed  Google Scholar 

  28. Liu X, Larouche S, Bowen P, Smith DR (2015) Clarifying the origin of third-harmonic generation from film-coupled nanostripes. Opt Express 23(15):19565–19574. https://doi.org/10.1364/OE.23.019565

    Article  CAS  PubMed  Google Scholar 

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Funding

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). https://doi.org/10.1007/s11468-021-01444-3

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