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

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.

Three-dimensional spatiotemporal tracking of nano-objects diffusing in water-filled optofluidic microstructured fiber

Three-dimensional (3D) tracking of nano-objects represents a novel pathway for understanding dynamic nanoscale processes within bioanalytics and life science. Here we demonstrate 3D tracking of diffusing 100 nm gold nanosphere within a water-filled optofluidic fiber via elastic light scattering–based position retrieval. Specifically, the correlation between intensity and position inside a region of a fiber-integrated microchannel has been used to decode the axial position from the scattered intensity, while image processing–based tracking was used in the image plane. The 3D trajectory of a diffusing gold nanosphere has been experimentally determined, while the determined diameter analysis matches expectations. Beside key advantages such as homogenous light-line illumination, low-background scattering, long observation time, large number of frames, high temporal and spatial resolution and compatibility with standard microscope, the particular properties of operating with water defines a new bioanalytical platform that is highly relevant for medical and life science applications.