Self-adjusted all-dielectric metasurfaces for deep ultraviolet femtosecond pulse generation.

The advantage of metasurfaces and nanostructures with a high nonlinear response is that they do not require phase matching, and the generated pulses are short in the time domain without additional pulse compression. However, the fabrication of large-scale planar structures by lithography-based methods is expensive, time consuming, and requires complicated preliminary simulations to obtain the most optimized geometry. Here, we propose a novel strategy for the self-assembled fabrication of large-scale resonant metasurfaces, where incident femtosecond laser pulses adjust the initial silicon films via specific surface deformation to be as resonant as possible for a given wavelength. The self-adjusting approach eliminates the necessity of multistep lithography and designing, because interference between the incident and the scattered parts of each laser pulse "imprints" resonant field distribution within the film. The self-adjusted metasurfaces demonstrate a high damage threshold (≈1012 W cm-2) and efficient frequency conversion from near-IR to deep UV. The conversion efficiency is up to 30-fold higher compared with nonresonant smooth Si films. The resulting metasurfaces allow for the generation of UV femtosecond laser pulses at a wavelength of 270 nm with a high peak and average power (≈105 W and ≈1.5 µW, respectively). The results pave the way to the creation of ultrathin nonlinear metadevices working at high laser intensities for efficient deep UV generation at the nanoscale.

Laser fabrication of crystalline silicon nanoresonators from an amorphous film for low-loss all-dielectric nanophotonics.

The concept of high refractive index subwavelength dielectric nanoresonators, supporting electric and magnetic optical resonance, is a promising platform for waveguiding, sensing, and nonlinear nanophotonic devices. However, high concentration of defects in the nanoresonators diminishes their resonant properties, which are crucially dependent on their internal losses. Therefore, it seems to be inevitable to use initially crystalline materials for fabrication of the nanoresonators. Here, we show that the fabrication of crystalline (low-loss) resonant silicon nanoparticles by femtosecond laser ablation of amorphous (high-loss) silicon thin films is possible. We apply two conceptually different approaches: recently proposed laser-induced transfer and a novel laser writing technique for large-scale fabrication of the crystalline nanoparticles. The crystallinity of the fabricated nanoparticles is proven by Raman spectroscopy and electron transmission microscopy, whereas optical resonant properties of the nanoparticles are studied using dark-field optical spectroscopy and full-wave electromagnetic simulations.