Nano-imprint lithography of broad-band and wide-angle antireflective structures for high-power lasers.

We demonstrate efficient anti reflection coatings based on adiabatic index matching obtained via nano-imprint lithography. They exhibit high total transmission, achromaticity (99.5% < T < 99.8% from 390 to 900 nm and 99% < T < 99.5% from 800 to 1600 nm) and wide angular acceptance (T > 99% up to 50 degrees). Our devices show high laser-induced damage thresholds in the sub-picosecond (>5 J/cm2 at 1030 nm, 500 fs), nanosecond (>150 J/cm2 at 1064 nm, 12 ns and >100 J/cm2 at 532 nm, 12 ns) regimes, and low absorption in the CW regime (<1.3 ppm at 1080 nm), close to those of the fused silica substrate.

Hyperuniform Monocrystalline Structures by Spinodal Solid-State Dewetting.

Materials featuring anomalous suppression of density fluctuations over large length scales are emerging systems known as disordered hyperuniform. The underlying hidden order renders them appealing for several applications, such as light management and topologically protected electronic states. These applications require scalable fabrication, which is hard to achieve with available top-down approaches. Theoretically, it is known that spinodal decomposition can lead to disordered hyperuniform architectures. Spontaneous formation of stable patterns could thus be a viable path for the bottom-up fabrication of these materials. Here, we show that monocrystalline semiconductor-based structures, in particular Si_{1-x}Ge_{x} layers deposited on silicon-on-insulator substrates, can undergo spinodal solid-state dewetting featuring correlated disorder with an effective hyperuniform character. Nano- to micrometric sized structures targeting specific morphologies and hyperuniform character can be obtained, proving the generality of the approach and paving the way for technological applications of disordered hyperuniform metamaterials. Phase-field simulations explain the underlying nonlinear dynamics and the physical origin of the emerging patterns.

Raman microscopy and infrared optical properties of SiGe Mie resonators formed on SiO2 via Ge condensation and solid state dewetting.

All-dielectric photonics is a rapidly developing field of optics and material science. The main interest at visible and near-infrared frequencies is light management using high-refractive-index Mie-resonant dielectric particles. Most work in this area of research focuses on exploiting Si-based particles. Here, we study monocrystalline Mie-resonant particles made of Ge-rich SiGe alloys with refractive index higher than that of Si. These islands are formed via solid state dewetting of SiGe flat layers by using two different processes: (i) dewetting of monocrystalline SiGe layers (60%-80% Ge content) obtained via Ge condensation of SiGe on silicon on insulator; and (ii) dewetting of a SiGe layer deposited via molecular beam epitaxy on silicon on insulator and ex situ Ge condensation, forming a Ge-rich shell surrounding a SiGe-core. Using high-spatial-resolution Raman microscopy we monitor Ge content x and strain ϵ of flat layers and SiGe-islands. We observe strain relaxation associated with formation of trading dislocations in the SiGe islands compared to the starting SiGe layers, as confirmed by TEM images. For initial high Ge concentration in the flat layers, the corresponding Ge content in the dewetted islands is lower, owing to diffusion of Si atoms from Si or SiO2 into SiGe islands. The Ge content also varies from particle to particle on the same sample. Size and shape of the dewetted particles depend on the fabrication process: thicker initial SiGe layers lead to larger particles. Samples with narrow island size distribution display rather sharp Mie resonances in the 1000-2500 nm spectral range. Larger islands display Mie resonances at longer wavelength. Positions of the resonances are in agreement with the theoretical calculations in the discrete dipole approximation.

Structure induced laminar vortices control anomalous dispersion in porous media.

Natural porous systems, such as soil, membranes, and biological tissues comprise disordered structures characterized by dead-end pores connected to a network of percolating channels. The release and dispersion of particles, solutes, and microorganisms from such features is key for a broad range of environmental and medical applications including soil remediation, filtration and drug delivery. Yet, owing to the stagnant and opaque nature of these disordered systems, the role of microscopic structure and flow on the dispersion of particles and solutes remains poorly understood. Here, we use a microfluidic model system that features a pore structure characterized by distributed dead-ends to determine how particles are transported, retained and dispersed. We observe strong tailing of arrival time distributions at the outlet of the medium characterized by power-law decay with an exponent of 2/3. Using numerical simulations and an analytical model, we link this behavior to particles initially located within dead-end pores, and explain the tailing exponent with a hopping across and rolling along the streamlines of vortices within dead-end pores. We quantify such anomalous dispersal by a stochastic model that predicts the full evolution of arrival times. Our results demonstrate how microscopic flow structures can impact macroscopic particle transport.

Scalable Disordered Hyperuniform Architectures via Nanoimprint Lithography of Metal Oxides.

Fabrication and scaling of disordered hyperuniform materials remain hampered by the difficulties in controlling the spontaneous phenomena leading to this novel kind of exotic arrangement of objects. Here, we demonstrate a hybrid top-down/bottom-up approach based on sol-gel dip-coating and nanoimprint lithography for the faithful reproduction of disordered hyperuniform metasurfaces in metal oxides. Nano- to microstructures made of silica and titania can be directly printed over several cm2 on glass and on silicon substrates. First, we describe the polymer mold fabrication starting from a hard master obtained via spontaneous solid-state dewetting of SiGe and Ge thin layers on SiO2. Then, we assess the effective disordered hyperuniform character of master and replica and the role of the thickness of the sol-gel layer on the metal oxide replicas and on the presence of a residual layer underneath. Finally, as a potential application, we show the antireflective character of titania structures on silicon. Our results are relevant for the realistic implementation over large scales of disordered hyperuniform nano- and microarchitectures made of metal oxides, thus opening their exploitation in the framework of wet chemical assembly.

Solid-State Dewetting Dynamics of Amorphous Ge Thin Films on Silicon Dioxide Substrates.

We report on the dewetting process, in a high vacuum environment, of amorphous Ge thin films on SiO2/Si (001). A detailed insight of the dewetting is obtained by in situ reflection high-energy electron diffraction and ex situ scanning electron microscopy. These characterizations show that the amorphous Ge films dewet into Ge crystalline nano-islands with dynamics dominated by crystallization of the amorphous material into crystalline nano-seeds and material transport at Ge islands. Surface energy minimization determines the dewetting process of crystalline Ge and controls the final stages of the process. At very high temperatures, coarsening of the island size distribution is observed.

Templated dewetting of single-crystal sub-millimeter-long nanowires and on-chip silicon circuits.

Large-scale, defect-free, micro- and nano-circuits with controlled inter-connections represent the nexus between electronic and photonic components. However, their fabrication over large scales often requires demanding procedures that are hardly scalable. Here we synthesize arrays of parallel ultra-long (up to 0.75 mm), monocrystalline, silicon-based nano-wires and complex, connected circuits exploiting low-resolution etching and annealing of thin silicon films on insulator. Phase field simulations reveal that crystal faceting and stabilization of the wires against breaking is due to surface energy anisotropy. Wires splitting, inter-connections and direction are independently managed by engineering the dewetting fronts and exploiting the spontaneous formation of kinks. Finally, we fabricate field-effect transistors with state-of-the-art trans-conductance and electron mobility. Beyond the first experimental evidence of controlled dewetting of patches featuring a record aspect ratio of [Formula: see text]1/60000 and self-assembled [Formula: see text]mm long nano-wires, our method constitutes a distinct and promising approach for the deterministic implementation of atomically-smooth, mono-crystalline electronic and photonic circuits.