Time-dependent nonlinear media, such as rapidly generated plasmas produced via laser ionization of gases, can increase the energy of individual laser photons and generate tunable high-order harmonic pulses. This phenomenon, known as photon acceleration, has traditionally required extreme-intensity laser pulses and macroscopic propagation lengths. Here, we report on a novel nonlinear material-an ultrathin semiconductor metasurface-that exhibits efficient photon acceleration at low intensities. We observe a signature nonlinear manifestation of photon acceleration: third-harmonic generation of near-infrared photons with tunable frequencies reaching up to ≈3.1ω. A simple time-dependent coupled-mode theory, found to be in good agreement with experimental results, is utilized to predict a new path towards nonlinear radiation sources that combine resonant upconversion with broadband operation.

Femtosecond-laser-assisted material restructuring employs extreme optical intensities to localize the ablation regions. To overcome the minimum feature size limit set by the wave nature of photons, there is a need for new approaches to tailored material processing at the nanoscale. Here, we report the formation of deeply-subwavelength features in silicon, enabled by localized laser-induced phase explosions in prefabricated silicon resonators. Using short trains of mid-infrared laser pulses, we demonstrate the controllable formation of high aspect ratio (>10:1) nanotrenches as narrow as [Formula: see text]. The trench geometry is shown to be scalable with wavelength, and controlled by multiple parameters of the laser pulse train, such as the intensity and polarization of each laser pulse and their total number. Particle-in-cell simulations reveal localized heating of silicon beyond its boiling point and suggest its subsequent phase explosion on the nanoscale commensurate with the experimental data. The observed femtosecond-laser assisted nanostructuring of engineered microstructures (FLANEM) expands the nanofabrication toolbox and opens exciting opportunities for high-throughput optical methods of nanoscale structuring of solid materials.

High harmonic generation (HHG) opens a window on the fundamental science of strong-field light-mater interaction and serves as a key building block for attosecond optics and metrology. Resonantly enhanced HHG from hot spots in nanostructures is an attractive route to overcoming the well-known limitations of gases and bulk solids. Here, we demonstrate a nanoscale platform for highly efficient HHG driven by intense mid-infrared laser pulses: an ultra-thin resonant gallium phosphide (GaP) metasurface. The wide bandgap and the lack of inversion symmetry of the GaP crystal enable the generation of even and odd harmonics covering a wide range of photon energies between 1.3 and 3 eV with minimal reabsorption. The resonantly enhanced conversion efficiency facilitates single-shot measurements that avoid material damage and pave the way to study the controllable transition between perturbative and non-perturbative regimes of light-matter interactions at the nanoscale.

Large scale laser facilities are needed to advance the energy frontier in high energy physics and accelerator physics. Laser plasma accelerators are core to advanced accelerator concepts aimed at reaching TeV electron electron colliders. In these facilities, intense laser pulses drive plasmas and are used to accelerate electrons to high energies in remarkably short distances. A laser plasma accelerator could in principle reach high energies with an accelerating length that is 1000 times shorter than in conventional RF based accelerators. Notionally, laser driven particle beam energies could scale beyond state of the art conventional accelerators. LPAs have produced multi GeV electron beams in about 20 cm with relative energy spread of about 2 percent, supported by highly developed laser technology. This validates key elements of the US DOE strategy for such accelerators to enable future colliders but extending best results to date to a TeV collider will require lasers with higher average power. While the per pulse energies envisioned for laser driven colliders are achievable with current lasers, low laser repetition rates limit potential collider luminosity. Applications will require rates of kHz to tens of kHz at Joules of energy and high efficiency, and a collider would require about 100 such stages, a leap from current Hz class LPAs. This represents a challenging 1000 fold increase in laser repetition rates beyond current state of the art. This whitepaper describes current research and outlook for candidate laser systems as well as the accompanying broadband and high damage threshold optics needed for driving future advanced accelerators.