Confined Phase Singularities Reveal the Spin-to-Orbital Angular Momentum Conversion of Sound Waves.

We identify an acoustic process in which the conversion of angular momentum between its spin and orbital form takes place. The interaction between an evanescent wave propagating at the interface of two immiscible fluids and an isolated droplet is considered. The elliptical motion of the fluid supporting the incident wave is associated with a simple state of spin angular momentum, a quantity recently introduced for acoustic waves in the literature. We experimentally observe that this field predominantly forces a directional wave transport circling the droplet's interior, revealing the existence of confined phase singularities. The circulation of the phase, around a singular point, is characteristic of angular momentum in its orbital form, thereby demonstrating the conversion mechanism. The numerical and experimental observations presented in this Letter have implications for the fundamental understanding of the angular momentum of acoustic waves, and for applications such as particle manipulation with radiation forces or torques, acoustic sensing and imaging.

A versatile technology for colloidal crystal transfer using parylene coatings and hydrosoluble polymers.

We propose a novel versatile colloidal crystal transfer technique compatible with a wide range of water-insoluble substrates regardless of their size, material, and wettability. There are no inherent limitations on colloidal particles material and size. The method possibilities are demonstrated via the colloidal transfer on quartz, glass substrates with a flat and curved surface, and via the fabrication of 3D colloidal structure with 5 overlaid colloidal monolayers. The process occurs at a room temperature in water and is independent from the illumination conditions, which makes it ideal for experimental manipulations with sensitive functional substrates. We performed the nanosphere photolithography process on a photosensitive substrate with a transferred colloidal monolayer. The metallized hexagonal arrays of nanopores demonstrated a clear resonant plasmonic behavior. We believe that due to its high integration possibilities the proposed transfer technique will find applications in a large-area surface nanotexturing, plasmonics, and will speed up a device fabrication process.

Experimental demonstration of negative refraction with 3D locally resonant acoustic metafluids.

Negative refraction of acoustic waves is demonstrated through underwater experiments conducted at ultrasonic frequencies on a 3D locally resonant acoustic metafluid made of soft porous silicone-rubber micro-beads suspended in a yield-stress fluid. By measuring the refracted angle of the acoustic beam transmitted through this metafluid shaped as a prism, we determine the acoustic index to water according to Snell's law. These experimental data are then compared with an excellent agreement to calculations performed in the framework of Multiple Scattering Theory showing that the emergence of negative refraction depends on the volume fraction [Formula: see text] of the resonant micro-beads. For diluted metafluid ([Formula: see text]), only positive refraction occurs whereas negative refraction is demonstrated over a broad frequency band with concentrated metafluid ([Formula: see text]).

Elaboration of soft porous ultrasound insulators.

A simple and easy way is proposed for the fabrication of a highly attenuating composite material for underwater acoustics. The approach involves the introduction of porous polymer beads into a polyurethane matrix. The porous beads are prepared through an emulsion-templating approach, and two different processes are used. The first one uses microfluidics to synthesize beads of controlled diameter and porosity. The control over the bead size allows the selection of the frequency range where the material exhibits the highest acoustic attenuation. The second one uses a double emulsion approach and allows for the production of much larger quantities of beads. Both approaches yield materials exhibiting much higher acoustic absorption than the one obtained using the most commonly used micro-balloon inclusion. We present both the synthesis procedures and the structural and acoustic characterizations of the beads and the final acoustic materials.

Flat acoustics with soft gradient-index metasurfaces.

Recently, metasurfaces have been proven to be effective and compact devices for the design of arbitrary wavefronts. Metasurfaces are planar metamaterials with a subwavelength thickness that allows wavefront shaping by introducing in-plane variations, namely, gradients, in the spatial wave response of these flat structures. Here we report a new class of acoustic gradient-index (GRIN) metasurfaces engineered from soft graded-porous silicone rubber with a high acoustic index for broadband ultrasonic three-dimensional wavefront shaping in water. The functionalities of these soft flat lenses are illustrated through various experiments, which demonstrate beam steering and beam focusing, as well as vortex beam generation in free space. These new GRIN metasurfaces may have important applications in various domains using designed ultrasonic fields (biomedical imaging, industrial non-destructive testing, contactless particle manipulation), since their fabrication is very straightforward with common polymer science engineering.

Nonreciprocal Thermal Material by Spatiotemporal Modulation.

The thermal properties of a material with a spatiotemporal modulation, in the form of a traveling wave, in both the thermal conductivity and the specific heat capacity are studied. It is found that these materials behave as materials with an internal convectionlike term that provides them with nonreciprocal properties, in the sense that the heat flux has different properties when it propagates in the same direction or in the opposite one to the modulation of the parameters. An effective medium description is presented which accurately describes the modulated material, and numerical simulations support this description and verify the nonreciprocal properties of the material. It is found that these materials are promising candidates for the design of thermal diodes and other advanced devices for the control of the heat flow at all scales.

Vapour sensitivity of an ALD hierarchical photonic structure inspired by Morpho.

The unique architecture of iridescent Morpho butterfly scales is known to exhibit different optical responses to various vapours. However, the mechanism behind this phenomenon is not fully quantitatively understood. This work reports on process developments in the micro-fabrication of a Morpho-inspired photonic structure in atomic layer deposited (ALD) materials in order to investigate the vapour optical sensitivity of such artificial nanostructures. By developing recipes for dry and wet etching of ALD oxides, we micro-fabricated two structures: one combining Al2O3 and TiO2, and the other combining Al2O3 and HfO2. For the first time, we report the optical response of such ALD Morpho-like structures measured under a controlled flow of either ethanol or isopropyl alcohol (IPA) vapour. In spite of the small magnitude of the effect, the results show a selective vapour response (depending on the materials used).

Damage evaluation in graphene underlying atomic layer deposition dielectrics.

Based on micro-Raman spectroscopy (µRS) and X-ray photoelectron spectroscopy (XPS), we study the structural damage incurred in monolayer (1L) and few-layer (FL) graphene subjected to atomic-layer deposition of HfO2 and Al2O3 upon different oxygen plasma power levels. We evaluate the damage level and the influence of the HfO2 thickness on graphene. The results indicate that in the case of Al2O3/graphene, whether 1L or FL graphene is strongly damaged under our process conditions. For the case of HfO2/graphene, µRS analysis clearly shows that FL graphene is less disordered than 1L graphene. In addition, the damage levels in FL graphene decrease with the number of layers. Moreover, the FL graphene damage is inversely proportional to the thickness of HfO2 film. Particularly, the bottom layer of twisted bilayer (t-2L) has the salient features of 1L graphene. Therefore, FL graphene allows for controlling/limiting the degree of defect during the PE-ALD HfO2 of dielectrics and could be a good starting material for building field effect transistors, sensors, touch screens and solar cells. Besides, the formation of Hf-C bonds may favor growing high-quality and uniform-coverage dielectric. HfO2 could be a suitable high-K gate dielectric with a scaling capability down to sub-5-nm for graphene-based transistors.

Soft 3D acoustic metamaterial with negative index.

Many efforts have been devoted to the design and achievement of negative-refractive-index metamaterials since the 2000s. One of the challenges at present is to extend that field beyond electromagnetism by realizing three-dimensional (3D) media with negative acoustic indices. We report a new class of locally resonant ultrasonic metafluids consisting of a concentrated suspension of macroporous microbeads engineered using soft-matter techniques. The propagation of Gaussian pulses within these random distributions of 'ultra-slow' Mie resonators is investigated through in situ ultrasonic experiments. The real part of the acoustic index is shown to be negative (up to almost - 1) over broad frequency bandwidths, depending on the volume fraction of the microbeads as predicted by multiple-scattering calculations. These soft 3D acoustic metamaterials open the way for key applications such as sub-wavelength imaging and transformation acoustics, which require the production of acoustic devices with negative or zero-valued indices.

Design of a fluorinated magneto-responsive material with tuneable ultrasound scattering properties.

In this work, we describe the preparation of emulsions of fluorinated ferrofluid droplets suspended in a yield-stress hydrogel (Bingham fluid) with potential applications for ultrasound (US) spectroscopy and imaging. Fluorinated ferrofluids were obtained using an original multi-step process leading to an appropriate suspension of magnetic nanoparticles (MNPs) coated by a layer of fluoroalkylsilane in fluorinated oil. The efficiency of the sol-gel coating reaction was assessed by several methods including infrared and X-ray photoelectron spectroscopy, small angle neutron scattering and magnetometry. The resulting suspension of silanized-MNPs behaves as a true fluorinated ferrofluid, remaining stable (i.e. a monophasic suspension of well dispersed MNPs) in magnetic inductions as high as 7 T. These ferrofluids were employed to prepare monodisperse emulsions in a Bingham gel using a robotic injection device. Using ultrasound spectroscopy, we show that the emulsion droplets behave as Mie-type acoustic wave resonators due to the high sound-speed contrast between the droplets and the matrix. When subjected to a magnetic field, the ferrofluid droplets elongate in the field direction, which in return modifies the acoustic response of the material. The resonance frequency peaks scale as the inverse of the emulsion droplet size encountered by the wave propagation vector. These results might open a new road towards the realisation of ultrasound contrast agents guided by magnetic fields and with a tuneable attenuation spectrum.

Impact of polydispersity on multipolar resonant scattering in emulsions.

The influence of size polydispersity on the resonant acoustic properties of dilute emulsions, made of fluorinated-oil droplets, is quantitatively investigated. Ultrasound attenuation and dispersion measurements on various samples with controlled size polydispersities, ranging from 1% to 13%, are found to be in excellent agreement with predictions based on the independent scattering approximation. By relating the particle-size distribution of the synthesized emulsions to the quality factor of the predicted multipolar resonances, the number of observable acoustic resonances is shown to be imposed by the sample polydispersity. These results are briefly discussed into the context of metamaterials for which scattering resonances are central to their effective properties.

Using dispersion equation for orthotropic media to model antiplane coherent wave propagation in cracked solids.

Attention is focused on the propagation of antiplane coherent wave obliquely incident on mutually parallel and randomly distributed cracks. A fundamental question in this study concerns the ability of describing the coherent wave propagation in all directions from the knowledge of the effective material properties along the effective principal directions, only. Its relevance is illustrated by considering two cases of coherent wave propagation: homogeneous and inhomogeneous waves. For both cases, the effective phase slownesses approximated from the dispersion equation specific for orthotropic homogeneous media are compared to reference results obtained from a direct calculation considering waves obliquely incident on cracks. This work reveals that the effective stiffnesses of this dispersion equation have to be dependent on the propagation direction of the incident wave in order to make this equation consistent.

Tuning Mie scattering resonances in soft materials with magnetic fields.

An original approach is proposed here to reversibly tune Mie scattering resonances occurring in random media by means of external low induction magnetic fields. This approach is valid for both electromagnetic and acoustic waves. The experimental demonstration is supported by ultrasound experiments performed on emulsions made of fluorinated ferrofluid spherical droplets dispersed in a Bingham fluid. We show that the electromagnet-induced change of droplet shape into prolate spheroids, with a moderate aspect ratio of 2.5, drastically affects the effective properties of the disordered medium. Its effective acoustic attenuation coefficient is shown to vary by a factor of 5, by controlling both the flux density and orientation of the applied magnetic field.

A comparative study of non-covalent encapsulation methods for organic dyes into silica nanoparticles.

Numerous luminophores may be encapsulated into silica nanoparticles (< 100 nm) using the reverse microemulsion process. Nevertheless, the behaviour and effect of such luminescent molecules appear to have been much less studied and may possibly prevent the encapsulation process from occurring. Such nanospheres represent attractive nanoplatforms for the development of biotargeted biocompatible luminescent tracers. Physical and chemical properties of the encapsulated molecules may be affected by the nanomatrix. This study examines the synthesis of different types of dispersed silica nanoparticles, the ability of the selected luminophores towards incorporation into the silica matrix of those nanoobjects as well as the photophysical properties of the produced dye-doped silica nanoparticles. The nanoparticles present mean diameters between 40 and 60 nm as shown by TEM analysis. Mainly, the photophysical characteristics of the dyes are retained upon their encapsulation into the silica matrix, leading to fluorescent silica nanoparticles. This feature article surveys recent research progress on the fabrication strategies of these dye-doped silica nanoparticles.

Almost ideal 1D water diffusion in imogolite nanotubes evidenced by NMR relaxometry.

The longitudinal proton relaxation rates R(1) of water diffusing inside synthetic aluminium silicate imogolite nanotubes are measured by fast field-cycling NMR for frequencies between 0.02 and 35 MHz at 25, 37 and 50 degrees C. We give analytical expressions of the dominant intermolecular dipolar spin-spin contribution to R(1) and to the transverse relaxation rate R(2). A remarkable variation of R(1) by more than two orders of magnitude is observed and shown to be close to the theoretical law, inversely proportional to the square root of the resonance frequency, which is characteristic of perfect molecular 1D diffusion. The physics of diffusion is discussed.

Lanthanide-chelate silica nanospheres as robust multicolor Vis-NIR tags.

Different lanthanide chelates have been simultaneously embedded in a silica matrix yielding bright dual-mode lanthanide doped nanospheres which are uniform in size distribution, tunable, photostable, and leakage free. Depending on the chelate combination, two color emission with a single light source or tunable emission with multiple sources is obtained.

Molecular dynamics study of hydrated imogolite. 2. Structure and dynamics of confined water.

The behaviour of water confined in an imogolite nanotube was studied by means of molecular dynamics simulations. The results of the study show an important difference between the interaction of water molecules with the internal and external surfaces of the nanotube. The analysis of the density profiles of confined molecules, of their spatial organisation, of the size of molecular clusters, of the lifetime of H-bonds in the system and of dynamical characteristics of molecules permits us to qualify the external imogolite surface as hydrophobic, whereas the internal surface reveals a hydrophilic character.

Control of the chemical cross-linking of gelatin by a thermosensitive polymer: example of switchable reactivity.

Chemical cross-linking of gelatin is achieved using a thermosensitive reactive copolymer based on N-isopropylacrylamide (NIPAM). The copolymer bears 5 mol % acrylic acid units which form amide bonds with the amino groups of gelatin in the presence of a water-soluble carbodiimide. The cross-linking reaction occurs only below the LCST congruent with 34 degrees C (lower critical solution temperature), i.e., when the copolymer is in the coil conformation. Above the LCST the copolymer adopts a globule conformation and its ability to react with gelatin is drastically reduced. By setting the temperature above or below the LCST it is possible to switch off or on the reactivity of the system and control the gelation process. The switch temperature can be set at the desired value by adjusting the composition of the thermosensitive copolymer.