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.

Engineering and detection of light scattering directionalities in dewetted nanoresonators through dark-field scanning microscopy.

Dewetted, SiGe nanoparticles have been successfully exploited for light management in the visible and near-infrared, although their scattering properties have been so far only qualitatively studied. Here, we demonstrate that the Mie resonances sustained by a SiGe-based nanoantenna under tilted illumination, can generate radiation patterns in different directions. We introduce a novel dark-field microscopy setup that exploits the movement of the nanoantenna under the objective lens to spectrally isolate Mie resonances contribution to the total scattering cross-section during the same measurement. The knowledge of islands' aspect ratio is then benchmarked by 3D, anisotropic phase-field simulations and contributes to a correct interpretation of the experimental data.

Engineering of the spin on dopant process on silicon on insulator substrate.

We report on a systematic analysis of phosphorus diffusion in silicon on insulator thin film via spin-on-dopant process (SOD). This method is used to provide an impurity source for semiconductor junction fabrication. The dopant is first spread into the substrate via SOD and then diffused by a rapid thermal annealing process. The dopant concentration and electron mobility were characterized at room and low temperature by four-probe and Hall bar electrical measurements. Time-of-flight-secondary ion mass spectroscopy was performed to estimate the diffusion profile of phosphorus for different annealing treatments. We find that a high phosphorous concentration (greater than 1020 atoms cm-3) with a limited diffusion of other chemical species and allowing to tune the electrical properties via annealing at high temperature for short time. The ease of implementation of the process, the low cost of the technique, the possibility to dope selectively and the uniform doping manufactured with statistical process control show that the methodology applied is very promising as an alternative to the conventional doping methods for the implementation of optoelectronic devices.

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.

Tailoring Strain and Morphology of Core-Shell SiGe Nanowires by Low-Temperature Ge Condensation.

Selective oxidation of the silicon element of silicon germanium (SiGe) alloys during thermal oxidation is a very important and technologically relevant mechanism used to fabricate a variety of microelectronic devices. We develop here a simple integrative approach involving vapor-liquid-solid (VLS) growth followed by selective oxidation steps to the construction of core-shell nanowires and higher-level ordered systems with scalable configurations. We examine the selective oxidation/condensation process under nonequilibrium conditions that gives rise to spontaneous formation of core-shell structures by germanium condensation. We contrast this strategy that uses reaction-diffusion-segregation mechanisms to produce coherently strained structures with highly configurable geometry and abrupt interfaces with growth-based processes which lead to low strained systems with nonuniform composition, three-dimensional morphology, and broad core-shell interface. We specially focus on SiGe core-shell nanowires and demonstrate that they can have up to 70% Ge-rich shell and 2% homogeneous strain with core diameter as small as 14 nm. Key elements of the building process associated with this approach are identified with regard to existing theoretical models. Moreover, starting from results of ab initio calculations, we discuss the electronic structure of these novel nanostructures as well as their wide potential for advanced device applications.

Templated Solid-State Dewetting of Thin Silicon Films.

Thin film dewetting can be efficiently exploited for the implementation of functionalized surfaces over very large scales. Although the formation of sub-micrometer sized crystals via solid-state dewetting represents a viable method for the fabrication of quantum dots and optical meta-surfaces, there are several limitations related to the intrinsic features of dewetting in a crystalline medium. Disordered spatial organization, size, and shape fluctuations are relevant issues not properly addressed so far. This study reports on the deterministic nucleation and precise positioning of Si- and SiGe-based nanocrystals by templated solid-state dewetting of thin silicon films. The dewetting dynamics is guided by pattern size and shape taking full control over number, size, shape, and relative position of the particles (islands dimensions and relative distances are in the hundreds nm range and fluctuate ≈11% for the volumes and ≈5% for the positioning).

Fabrication of core-shell nanostructures via silicon on insulator dewetting and germanium condensation: towards a strain tuning method for SiGe-based heterostructures in a three-dimensional geometry.

We report on a novel method for the implementation of core-shell SiGe-based nanocrystals combining silicon on insulator dewetting in a molecular beam epitaxy reactor with an ex situ Ge condensation process. With an in situ two-step process (annealing and Ge deposition) we produce two families of islands on the same sample: Si-rich, formed during the first step and, all around them, Ge-rich formed after Ge deposition. By increasing the amount of Ge deposited on the annealed samples from 0 to 18 monolayers, the islands' shape in the Si-rich zones can be tuned from elongated and flat to more symmetric and with a larger vertical aspect ratio. At the same time, the spatial extension of the Ge-rich zones is progressively increased as well as the Ge content in the islands. Further processing by ex situ rapid thermal oxidation results in the formation of a core-shell composition profile in both Si and Ge-rich zones with atomically sharp heterointerfaces. The Ge condensation induces a Ge enrichment of the islands' shell of up to 50% while keeping a pure Si core in the Si-rich zones and a ∼25% SiGe alloy in the Ge-rich ones. The large lattice mismatch between core and shell, the absence of dislocations and the islands' monocrystalline nature render this novel class of nanostructures a promising device platform for strain-based band-gap engineering. Finally, this method can be used for the implementation of ultralarge scale meta-surfaces with dielectric Mie resonators for light manipulation at the nanoscale.

Back-propagation optimization and multi-valued artificial neural networks for highly vivid structural color filter metasurfaces.

We introduce a novel technique for designing color filter metasurfaces using a data-driven approach based on deep learning. Our innovative approach employs inverse design principles to identify highly efficient designs that outperform all the configurations in the dataset, which consists of 585 distinct geometries solely. By combining Multi-Valued Artificial Neural Networks and back-propagation optimization, we overcome the limitations of previous approaches, such as poor performance due to extrapolation and undesired local minima. Consequently, we successfully create reliable and highly efficient configurations for metasurface color filters capable of producing exceptionally vivid colors that go beyond the sRGB gamut. Furthermore, our deep learning technique can be extended to design various pixellated metasurface configurations with different functionalities.

Polariton condensation in photonic molecules.

We report on polariton condensation in photonic molecules formed by two coupled micropillars. We show that the condensation process is strongly affected by the interaction with the cloud of uncondensed excitons and thus strongly depends on the exact localization of these excitons within the molecule. Under symmetric excitation conditions, condensation is triggered on both binding and antibinding polariton states of the molecule. On the opposite, when the excitonic cloud is injected in one of the two pillars, condensation on a metastable state is observed and a total transfer of the condensate into one of the micropillars can be achieved. Our results highlight the crucial role played by relaxation kinetics in the condensation process.

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.

Polarization Anisotropies in Strain-Free, Asymmetric, and Symmetric Quantum Dots Grown by Droplet Epitaxy.

We provide an extensive and systematic investigation of exciton dynamics in droplet epitaxial quantum dots comparing the cases of (311)A, (001), and (111)A surfaces. Despite a similar s-shell exciton structure common to the three cases, the absence of a wetting layer for (311)A and (111)A samples leads to a larger carrier confinement compared to (001), where a wetting layer is present. This leads to a more pronounced dependence of the binding energies of s-shell excitons on the quantum dot size and to the strong anti-binding character of the positive-charged exciton for smaller quantum dots. In-plane geometrical anisotropies of (311)A and (001) quantum dots lead to a large electron-hole fine interaction (fine structure splitting (FSS) ∼100 µeV), whereas for the three-fold symmetric (111)A counterpart, this figure of merit is reduced by about one order of magnitude. In all these cases, we do not observe any size dependence of the fine structure splitting. Heavy-hole/light-hole mixing is present in all the studied cases, leading to a broad spread of linear polarization anisotropy (from 0 up to about 50%) irrespective of surface orientation (symmetry of the confinement), fine structure splitting, and nanostructure size. These results are important for the further development of ideal single and entangled photon sources based on semiconductor quantum dots.

Quasi-Guided Modes in Titanium Dioxide Arrays Fabricated via Soft Nanoimprint Lithography.

Reversible quasi-guided modes (QGMs) are observed in titanium dioxide (TiO2) metasurface arrays fabricated via soft nanoimprint lithography. A TiO2 layer between the nanopillar array and the substrate can facilitate the propagation of QGMs. This layer is porous, allowing for the tuning of the layer properties by incorporating another material. The presence of the QGMs is strongly dependent on the refractive index of the TiO2 layer. QGMs are not supported if the refractive index of the porous TiO2 is too low. It is demonstrated that after depositing R6G on the array QGMs can be observed as very strong and narrow reflectance peaks and transmittance dips. Furthermore, as the second material can penetrate through the pores into the layer it can experience the regions of high field enhancement associated with the QGMs. These results are of interest for a wide range of applications including but not limited to sensing, nonlinear optics, and emission control.

New Strategies for Engineering Tensile Strained Si Layers for Novel n-Type MOSFET.

We report a novel approach for engineering tensely strained Si layers on a relaxed silicon germanium on insulator (SGOI) film using a combination of condensation, annealing, and epitaxy in conditions specifically chosen from elastic simulations. The study shows the remarkable role of the SiO2 buried oxide layer (BOX) on the elastic behavior of the system. We show that tensely strained Si can be engineered by using alternatively rigidity (at low temperature) and viscoelasticity (at high temperature) of the SiO2 substrate. In these conditions, we get a Si strained layer perfectly flat and free of defects on top of relaxed Si1-xGex. We found very specific annealing conditions to relax SGOI while keeping a homogeneous Ge concentration and an excellent thickness uniformity resulting from the viscoelasticity of SiO2 at this temperature, which would allow layer-by-layer matter redistribution. Remarkably, the Si layer epitaxially grown on relaxed SGOI remains fully strained with -0.85% tensile strain. The absence of strain sharing (between Si1-xGex and Si) is explained by the rigidity of the Si1-xGex/BOX interface at low temperature. Elastic simulations of the real system show that, because of the very specific elastic characteristics of SiO2, there are unique experimental conditions that both relax Si1-xGex and keep Si strained. Various epitaxial processes could be revisited in light of these new results. The generic and simple process implemented here meets all the requirements of the microelectronics industry and should be rapidly integrated in the fabrication lines of large multifinger 2.5 V n-type MOSFET on SOI used for RF-switch applications and for many other applications.

Enhanced Refractive Index Sensitivity through Combining a Sol-Gel Adsorbate with a TiO2 Nanoimprinted Metasurface for Gas Sensing.

We combine a gas-adsorbent microporous hybrid silica layer and a dense TiO2 Mie resonator array (metasurface), both obtained by sol-gel deposition and nanoimprint lithography, to form nanocomposite systems with high sensitivity for refractive index (RI) variations induced by gas adsorption. Using optical transduction based on direct specular reflection, we show spectral shifts of 4470 nm/RIU corresponding to 0.2 nm/ppm gas (air concentration) and reflection intensity changes of R* = 17 (R/RIU) and 0.55 × 10-3 R/ppm (air concentration). The metasurface is composed of hexagonally arranged TiO2 nanopillar arrays, whereas the surrounding sensitive material is a class II microporous hybrid silica, containing methyl and phenyl covalently bonded organic functions. This hybrid layer shows efficient adsorption capability of volatile organic molecules such as isopropanol, which is used to induce slight variations of RI around the TiO2 antennas. Specular reflectance variations at 45° incidence and refractive index measurements are performed using a spectroscopic ellipsometer. The presence of the titania metasurface enhances the signal by almost an order of magnitude with respect to the 2D counterpart (simulated as an effective medium approximation) and is attributed to the antenna effect, enhancing the interaction of the confined electromagnetic wave with the sensitive microporous medium. This sol-gel nanocomposite system presents many advantages such as high throughput and low-cost elaboration of elements and a high chemical, mechanical, and thermal resistance, ensuring high stability as a potential gas-sensitive nanocomposite layer for long periods. This work is a case study of improving the sensitivity of sol-gel gas-sensitive materials in optical transduction, which will be exploited in further works to develop artificial noses.

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.

Exciton Dynamics in Droplet Epitaxial Quantum Dots Grown on (311)A-Oriented Substrates.

Droplet epitaxy allows the efficient fabrication of a plethora of 3D, III-V-based nanostructures on different crystalline orientations. Quantum dots grown on a (311)A-oriented surface are obtained with record surface density, with or without a wetting layer. These are appealing features for quantum dot lasing, thanks to the large density of quantum emitters and a truly 3D lateral confinement. However, the intimate photophysics of this class of nanostructures has not yet been investigated. Here, we address the main optical and electronic properties of s-shell excitons in individual quantum dots grown on (311)A substrates with photoluminescence spectroscopy experiments. We show the presence of neutral exciton and biexciton as well as positive and negative charged excitons. We investigate the origins of spectral broadening, identifying them in spectral diffusion at low temperature and phonon interaction at higher temperature, the presence of fine interactions between electron and hole spin, and a relevant heavy-hole/light-hole mixing. We interpret the level filling with a simple Poissonian model reproducing the power excitation dependence of the s-shell excitons. These results are relevant for the further improvement of this class of quantum emitters and their exploitation as single-photon sources for low-density samples as well as for efficient lasers for high-density samples.

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.

Capillary-driven elastic attraction between quantum dots.

We present a novel self-assembly route to align SiGe quantum dots. By a combination of theoretical analyses and experimental investigation, we show that epitaxial SiGe quantum dots can cluster in ordered closely packed assemblies, revealing an attractive phenomenon. We compute nucleation energy barriers, accounting for elastic effects between quantum dots through both elastic energy and strain-dependent surface energy. If the former is mostly repulsive, we show that the decrease in the surface energy close to an existing island reduces the nucleation barrier. It subsequently increases the probability of nucleation close to an existing island, and turns out to be equivalent to an effective attraction between dots. We show by Monte-Carlo simulations that this effect describes well the experimental results, revealing a new mechanism ruling self-organisation of quantum dots. Such a generic process could be observed in various heterogeneous systems and could pave the way for a wide range of applications.