We show that scattering from a single gold nanoparticle is saturable for the first time. Wavelength-dependent study reveals that the saturation behavior is governed by depletion of surface plasmon resonance, not the thermal effect. We observed interesting flattening of the point spread function of scattering from a single nanoparticle due to saturation. By extracting the saturated part of scattering via temporal modulation, we achieve λ/8 point spread function in far-field imaging with unambiguous separation of adjacent particles.

Nonlinear optical interaction is crucial to alloptical signal processing. In metallic nanostructures, both linear and nonlinear optical interactions can be greatly enhanced by surface plasmon resonance (SPR). In the last few decades, saturation and reverse saturation of absorption in plasmonic materials have been unraveled. It is known that scattering is one of the fundamental light−matter interactions and is particularly strong in metallic nanoparticles due to SPR. However, previous methods measure response from ensemble of nanoparticles and did not characterize scattering on a single particle basis. Here we report that backscattering from an isolated gold nanoparticle exhibits not only saturation, but also reverse saturation. Wavelength-dependent and intensitydependent studies reveal that nonlinear scattering is dominated by SPR and shares a similar physical origin with nonlinear absorption. The reversibility and repeatability of saturable scattering (SS) and reverse saturable scattering (RSS) are validated via repetitive excitation on the same set of particles. Compared to fluorescence, our novel discovery of single-particle-based SS and RSS does not suffer from bleaching and can be used as a more robust contrast agent for optical microscopy. Under a reflection confocal microscope, interesting point-spread functions are observed, with full-width-of-half-maximum of central and side lobes reduced to λ/5 and λ/13, showing great potential for superresolution microscopy.

Because of their exceptional local-field enhancement and ultrasmall mode volume, plasmonic components can integrate photonics and electronics at nanoscale, and active control of plasmons is the key. However, all-optical modulation of plasmonic response with nanometer mode volume and unity modulation depth is still lacking. Here we show that scattering from a plasmonic nanoparticle, whose volume is smaller than 0.001 μm3, can be optically switched off with less than 100 μW power. Over 80% modulation depth is observed, and shows no degradation after repetitive switching. The spectral bandwidth approaches 100 nm. The underlying mechanism is suggested to be photothermal effects, and the effective single-particle nonlinearity reaches nearly 10−9 m2/W, which is to our knowledge the largest record of metallic materials to date. As a novel application, the non-bleaching and unlimitedly switchable scattering is used to enhance optical resolution to λ/5 (λ/9 after deconvolution), with 100-fold less intensity requirement compared to similar superresolution techniques. Our work not only opens up a new field of ultrasmall all-optical control based on scattering from a single nanoparticle, but also facilitates superresolution imaging for long-term observation.

Recently, we discovered, for the first time, reverse saturable scattering in a single gold nanoparticle. When incident intensity increases, the scattering intensity dependence of 80-nm gold nanoparticles evolves from linear, to saturation, and to reverse saturation sequentially. The intensity dependence in reverse saturable scattering region is significantly steeper than that in the linear region. With the aid of a confocal microscope, the full width half maximum of the single-particle point spread function can be reduced down to 80 nm, which is beyond the diffraction limit. Our finding shows great potential for superresolution imaging application without bleaching.

No abstract