Light-induced symmetry breaking for enhancing second-harmonic generation from an ultrathin plasmonic nanocavity

Guang-Can Li, Dangyuan Lei (), Meng Qiu, Wei Jin, Sheng Lan and Anatoly V. Zayats ()
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Guang-Can Li: Guangdong Provincial Key Laboratory of Nanophotonic Functional Materials and Devices, School of Information and Optoelectronic Science and Engineering, South China Normal University
Dangyuan Lei: City University of Hong Kong
Meng Qiu: The Hong Kong Polytechnic University
Wei Jin: The Hong Kong Polytechnic University
Sheng Lan: Guangdong Provincial Key Laboratory of Nanophotonic Functional Materials and Devices, School of Information and Optoelectronic Science and Engineering, South China Normal University
Anatoly V. Zayats: King’s College London, Strand

Nature Communications, 2021, vol. 12, issue 1, 1-8

Abstract: Abstract Efficient frequency up-conversion of coherent light at the nanoscale is highly demanded for a variety of modern photonic applications, but it remains challenging in nanophotonics. Surface second-order nonlinearity of noble metals can be significantly boosted up by plasmon-induced field enhancement, however the related far-field second-harmonic generation (SHG) may also be quenched in highly symmetric plasmonic nanostructures despite huge near-field amplification. Here, we demonstrate that the SHG from a single gold nanosphere is significantly enhanced when tightly coupled to a metal film, even in the absence of a plasmon resonance at the SH frequency. The light-induced electromagnetic asymmetry in the nanogap junction efficiently suppresses the cancelling of locally generated SHG fields and the SH emission is further amplified through preferential coupling to the bright, bonding dipolar resonance mode of the nanocavity. The far-field SHG conversion efficiency of up to $$3.56\times 10^{-7}$$ 3.56 × 1 0 − 7 W−1 is demonstrated from a single gold nanosphere of 100 nm diameter, two orders of magnitude higher than for complex double-resonant plasmonic nanostructures. Such highly efficient SHG from a metal nanocavity also constitutes an ultrasensitive nonlinear nanoprobe to map the distribution of longitudinal vectorial light fields in nanophotonic systems.

Date: 2021
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DOI: 10.1038/s41467-021-24408-x

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