International audiencePlasmonic dimer nanoantennas can significantly boost the electric field strength in the gap region, allowing for a modification of the feed gap geometry by femtosecond laser illumination. Using resonant bowtie antennas to enhance the electric field of a low-fluence femtosecond oscillator, here we experimentally demonstrate highly localized reshaping of the antennas, resulting in a self-optimization of the antenna shape. From high-resolution scanning electron micrographs and two-dimensional energy dispersive x-ray maps, we analyze the near-field enhanced subwavelength ablation at the nanotips and the resulting deposition of ablated materials in the feed gap. The dominant ablation mechanism is attributed to the nonthermal transient unbonding of atoms and electrostatic acceleration of ions. This process is driven by surface plasmon enhanced electron emission, with subsequent acceleration in the vacuum. This ablation is impeded in the presence of an ambient gas. A maximum of sixfold enhancement of the third-harmonic yield is observed during the reshaping process

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We employ a broadband Ti:sapphire femtosecond oscillator to simultaneously launch two localized surface plasmon modes in rectangular plasmonic nanoholes. The resonant frequencies of these two modes match well with our laser spectrum. As a result, the nanoholes do not only efficiently boost the third harmonic radiation intensity, but also significantly broaden the harmonic's bandwidth, producing a nanoscale deep-ultraviolet light source in the range of 240 to 300 nm. Due to the involvement of two modes, the third harmonic beam becomes elliptically polarized and reaches its maximum intensity when laser polarization direction is 60°with respect to the long edges, rather than the commonly used 90°.

We experimentally investigate the interaction between hybrid-morphology gold optical antennas and a fewcycle Ti:sapphire laser up to ablative intensities, demonstrating rich nonlinear plasmonic effects and promising applications in coherent frequency upconversion and nanofabrication technology. The two-dimensional array of hybrid antennas consists of elliptical apertures combined with bowties in its minor axis. The plasmonic resonance frequency of the bowties is red-shifted with respect to the laser central frequency and thus mainly enhances the third harmonic spectrum at long wavelengths. The gold film between two neighboring elliptical apertures forms an hourglass-shaped structure, which acts as a "plasmonic lens" and thus strongly reinforces surface currents into a small area. This enhanced surface current produces a rotating magnetic field that deeply penetrates into the substrate. At resonant frequency, the magnetic field is further intensified by the bowties. The resonant frequency of the hourglass is blueshifted with respect to the laser central frequency. Consequently, it spectacularly extends the third harmonic spectrum toward short wavelengths. The resultant third harmonic signal ranges from 230 to 300 nm, much broader than the emission from a sapphire crystal. In addition, the concentration of surface current within the neck of the hourglass antenna results in a structural modification through laser ablation, producing sub-10 nm sharp metallic gaps. Moreover, after laser illumination the optical field hotspots are imprinted around the antennas, allowing us to confirm the subwavelength enhancement of the electric near-field intensity.