23 September 2016 Nonlinear scattering in plasmonic nanostructures
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Nonlinear phenomena provide novel light manipulation capabilities and innovative applications. Recently, we discovered nonlinear saturation on single-particle scattering of gold nanospheres by continuous-wave laser excitation and innovatively applied to improve microscopic resolution down to λ/8. However, the nonlinearity was limited to the green-orange plasmonic band of gold nanosphere, and the underlying mechanism has not yet been fully understood. In this work, we demonstrated that nonlinear scattering exists for various material/geometry combinations, thus expanding the applicable wavelength range. For near-infrared, gold nanorod is used, while for blue-violet, silver nanospheres are adopted. In terms of mechanism, the nonlinearity may originate from interband/intraband absorption, hot electron, or hot lattice, which are spectrally mixed in the case of gold nanosphere. For gold nanorod and silver nanosphere, nonlinear scattering occurs at plasmonic resonances, which are spectrally far from interband/intraband absorptions, so they are excluded. We found that the nonlinear index is much larger than possible contributions from hot electrons in literature. Therefore, we conclude that hot lattice is the major mechanism. In addition, we propose that similar to z-scan, which is the standard method to characterize nonlinearity of a thin sample, laser scanning microscopy should be adopted as the standard method to characterize nonlinearity from a nanostructure. Our work not only provides the physical mechanism of the nonlinear scattering, but also paves the way toward multi-color superresolution imaging based on non-bleaching plasmonic scattering.
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Shi-Wei Chu, Shi-Wei Chu, "Nonlinear scattering in plasmonic nanostructures", Proc. SPIE 9921, Plasmonics: Design, Materials, Fabrication, Characterization, and Applications XIV, 99210D (23 September 2016); doi: 10.1117/12.2238382; https://doi.org/10.1117/12.2238382

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