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Third-harmonic-upconversion enhancement from a single semiconductor nanoparticle coupled to a plasmonic antenna

Nature Nanotechnology volume 9, pages 290–294 (2014)Cite this article

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Abstract

The ability to convert low-energy quanta into a quantum of higher energy is of great interest for a variety of applications, including bioimaging1, drug delivery2 and photovoltaics3. Although high conversion efficiencies can be achieved using macroscopic nonlinear crystals, upconverting light at the nanometre scale remains challenging because the subwavelength scale of materials prevents the exploitation of phase-matching processes4. Light–plasmon interactions that occur in nanostructured noble metals have offered alternative opportunities for nonlinear upconversion of infrared light, but conversion efficiency rates remain extremely low due to the weak penetration of the exciting fields into the metal5. Here, we show that third-harmonic generation from an individual semiconductor indium tin oxide nanoparticle is significantly enhanced when coupled within a plasmonic gold dimer. The plasmonic dimer acts as a receiving optical antenna6, confining the incident far-field radiation into a near field localized at its gap; the indium tin oxide nanoparticle located at the plasmonic dimer gap acts as a localized nonlinear transmitter upconverting three incident photons at frequency ω into a photon at frequency 3ω. This hybrid nanodevice provides third-harmonic-generation enhancements of up to 106-fold compared with an isolated indium tin oxide nanoparticle, with an effective third-order susceptibility up to 3.5 × 103 nm2 V−2 and conversion efficiency of 0.0007%. We also show that the upconverted third-harmonic emission can be exploited to probe the near-field intensity at the plasmonic dimer gap.

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Figure 1: Nonlinear upconversion nanosystem.
Figure 2: Three-photon upconversion enhancement from a single ITO nanoparticle decorated with a plasmonic dimer.
Figure 3: Probing plasmonic hot spots with a nanoscale nonlinear particle.

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Acknowledgements

The authors thank A. Rakovich for fabrication of preliminary samples, Y. Sonnefraud for help with sample characterization and V. Giannini and A. I. Fernández-Domínguez for discussions. This work was funded by the Engineering and Physical Sciences Research Council (EPSRC) through the Active Plasmonics programme, the Leverhulme Trust, the US Army International Technology Centre Atlantic (USAITC-A) and the Office of Naval Research (ONR and ONR Global). M.N-C. is supported by an Imperial College Junior Research Fellowship.

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  1. Heykel Aouani and Mohsen Rahmani: These authors contributed equally to this work

Authors and Affiliations

  1. Department of Physics, The Blackett Laboratory, Imperial College London, London, SW7 2AZ, UK

    Heykel Aouani, Mohsen Rahmani & Stefan A. Maier

  2. Department of Electrical and Electronic Engineering, Optical and Semiconductor Devices Group, Imperial College London, London, SW7 2BT, UK

    Miguel Navarro-Cía

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  1. Heykel Aouani
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Contributions

H.A. and S.A.M. conceived and supervised the project. M.N-C. provided the numerical work, M.R. fabricated the samples and H.A. performed the experiments. H.A. wrote the manuscript. All authors participated in data processing, analysis, discussions and manuscript preparation.

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Correspondence to Heykel Aouani.

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The authors declare no competing financial interests.

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Aouani, H., Rahmani, M., Navarro-Cía, M. et al. Third-harmonic-upconversion enhancement from a single semiconductor nanoparticle coupled to a plasmonic antenna. Nature Nanotech 9, 290–294 (2014). https://doi.org/10.1038/nnano.2014.27

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