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Title: Light-induced symmetry breaking for enhancing second-harmonic generation from an ultrathin plasmonic nanocavity
Authors: Li, GC 
Lei, D 
Qiu, M 
Jin, W 
Lan, S
Zayats, AV
Issue Date: 2021
Source: Nature communications, 2021, v. 12, 4326
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 × 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.
Publisher: Nature Publishing Group
Journal: Nature communications 
EISSN: 2041-1723
DOI: 10.1038/s41467-021-24408-x
Rights: © The Author(s) 2021
Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
The following publication Li, G. C., Lei, D., Qiu, M., Jin, W., Lan, S., & Zayats, A. V. (2021). Light-induced symmetry breaking for enhancing second-harmonic generation from an ultrathin plasmonic nanocavity. Nature Communications, 12(1), 1-8 is available at https://doi.org/10.1038/s41467-021-24408-x
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