Suppressing torsional buckling in auxetic meta-shells.

Take a thin cylindrical shell and twist it; it will buckle immediately. Such unavoidable torsional buckling can lead to systemic failure, for example by disrupting the blood flow through arteries. In this study, we prevent this torsional buckling instability using a combination of auxeticity and orthotropy in cylindrical metamaterial shells with a holey pattern. When the principal axes of the orthotropic meta-shell are relatively aligned with that of the compressive component of the applied stress during twisting, the meta-shell uniformly shrinks in the radial direction as a result of a local buckling instability. This shrinkage coincides with a softening-stiffening transition that leads to ordered stacking of unit cells along the compressive component of the applied stress. These transitions due to local instabilities circumvent the usual torsional instability even under a large twist angle. This study highlights the potential of tailoring anisotropy and programming instabilities in metamaterials, with potential applications in designing mechanical elements for soft robotics, biomechanics or fluidics. As an example of such applications, we demonstrate soft torsional compressor for generating pulsatile flows through a torsion release mechanism.

The effect of decoupling humidity control on aerosol drug delivery during HFNC for infants.

BACKGROUND: Aerosol therapy is commonly used during treatment with high-flow nasal cannula (HFNC) in the intensive care unit (ICU). Heated humidification inside the HFNC tubing circuit leads to unwanted condensation, which may greatly limit the efficiency of drug delivery. In this study, we aimed to investigate whether a novel humidification system, which decouples temperature and humidity control, can improve the delivered dose. METHODS: In a bench study setup, fluorescein sodium solution was nebulized using a vibrating-mesh nebulizer in an infant HFNC circuit to measure the delivered dose, with a conventional versus a novel decoupled humidifier. The deposition of fluorescein inside each breathing circuit component and a final collection filter at the end of the nasal cannula was collected and quantified with a UV-vis spectrometer. Droplet sizes at different sections of the breathing circuit were measured by laser diffraction. Three air flow rates: 5, 10 and 15 L/min, and two nebulizer positions: (1) at the humidifier and (2) after the inspiratory tube, were tested. RESULTS: The delivered dose decreased with increasing flow rate for the conventional setup and was higher when the nebulizer was placed after the inspiratory tube. Turning off the conventional humidifier 10 minutes before and during nebulization did not improve the delivered dose. The decoupled humidifier achieved a significantly higher (p = .002) delivered dose than the conventional setup. The highest delivered dose obtained by the decoupled humidifier was 62.4% when the nebulizer was placed after the humidifier, while the highest dose obtained for the conventional humidifier was 36.3% by placing the nebulizer after the inspiratory tube. CONCLUSIONS: In this bench study, we found that the delivered dose for an infant HFNC nebulization setup could be improved significantly by decoupling temperature and humidity control inside the HFNC circuit, as it reduced drug deposition inside the breathing circuit.

Ductile-to-brittle transition and yielding in soft amorphous materials: perspectives and open questions.

Soft amorphous materials are viscoelastic solids ubiquitously found around us, from clays and cementitious pastes to emulsions and physical gels encountered in food or biomedical engineering. Under an external deformation, these materials undergo a noteworthy transition from a solid to a liquid state that reshapes the material microstructure. This yielding transition was the main theme of a workshop held from January 9 to 13, 2023 at the Lorentz Center in Leiden. The manuscript presented here offers a critical perspective on the subject, synthesizing insights from the various brainstorming sessions and informal discussions that unfolded during this week of vibrant exchange of ideas. The result of these exchanges takes the form of a series of open questions that represent outstanding experimental, numerical, and theoretical challenges to be tackled in the near future.

Thermal Properties of Athermal Granular Materials.

Dry granular materials consist of a vast ensemble of discrete solid particles interacting through complex frictional forces at the contact points. The particles are so large that these systems are believed to be completely athermal. Here, we arrest the dynamics of a flowing granular material in a steady-state-flow configuration, enabling an isolated examination of aging at the particle contacts without granular rearrangements. Our findings reveal that the evolution of interparticle forces within the arrested athermal granular network results in the spontaneous increase of the system's yield stress. This strengthening process is logarithmic in time with a rate that depends on the temperature. We demonstrate that the material's stress relaxation exhibits similar time- and temperature-dependent behavior, suggesting a shared origin for aging and stress relaxation in these systems governed by thermal molecular processes at the scale of the grain contacts.

Electroless Ionization Mass Spectrometry Using a Compact Electrokinetic Ionization Source.

We introduce a new ionization technique for compact, portable mass spectrometers. It consists of a syringe with sample liquid capped by a self-ionizing spray nozzle containing a microfabricated nozzle chip. Interaction of the sample liquid with the nozzle wall results in electrical charging without the need for electronics. Elaborate cleaning procedures are redundant when disposable syringes and mass-fabricated spray nozzles are used. This self-named electroless spray ionization (ELI) technique shows comparable performance to conventional ionization techniques. In contrast to commonly used electrospray ionization, ELI exhibits excellent ionization efficiency for low-conductive solutions such as water or acetonitrile. Due to its compact size and the absence of high-voltage electronics, it can also be readily integrated in other ionization sources. Besides reviewing the main properties of ELI, we showcase the technique's potential for two on-site, ambient mass spectroscopy applications: perfume fingerprinting and fast screening of fungicides on citrus fruits.

Molecular Probing of the Microscopic Pressure at Contact Interfaces.

Obtaining insights into friction at the nanoscopic level and being able to translate these into macroscopic friction behavior in real-world systems is of paramount importance in many contexts, ranging from transportation to high-precision technology and seismology. Since friction is controlled by the local pressure at the contact it is important to be able to detect both the real contact area and the nanoscopic local pressure distribution simultaneously. In this paper, we present a method that uses planarizable molecular probes in combination with fluorescence microscopy to achieve this goal. These probes, inherently twisted in their ground states, undergo planarization under the influence of pressure, leading to bathochromic and hyperchromic shifts of their UV-vis absorption band. This allows us to map the local pressure in mechanical contact from fluorescence by exciting the emission in the long-wavelength region of the absorption band. We demonstrate a linear relationship between fluorescence intensity and (simulated) pressure at the submicron scale. This relationship enables us to experimentally depict the pressure distribution in multiasperity contacts. The method presented here offers a new way of bridging friction studies of the nanoscale model systems and practical situations for which surface roughness plays a crucial role.

Perturbation-induced granular fluidization as a model for remote earthquake triggering.

Studying the effect of mechanical perturbations on granular systems is crucial for understanding soil stability, avalanches, and earthquakes. We investigate a granular system as a laboratory proxy for fault gouge. When subjected to a slow shear, granular materials typically exhibit a stress overshoot before reaching a steady state. We find that short seismic pulses can reset a granular system flowing in steady state so that the stress overshoot is regenerated. This feature is shown to determine the stability of the granular system under different applied stresses in the wake of a perturbation pulse and the resulting dynamics when it fails. Using an analytical aging-rejuvenation model for describing the overshoot response, we show that our laboratory-derived theoretical framework can quantitatively explain data from two fault slip events triggered by seismic waves.

Elucidating the role of water in collagen self-assembly by isotopically modulating collagen hydration.

Water is known to play an important role in collagen self-assembly, but it is still largely unclear how water-collagen interactions influence the assembly process and determine the fibril network properties. Here, we use the H[Formula: see text]O/D[Formula: see text]O isotope effect on the hydrogen-bond strength in water to investigate the role of hydration in collagen self-assembly. We dissolve collagen in H[Formula: see text]O and D[Formula: see text]O and compare the growth kinetics and the structure of the collagen assemblies formed in these water isotopomers. Surprisingly, collagen assembly occurs ten times faster in D[Formula: see text]O than in H[Formula: see text]O, and collagen in D[Formula: see text]O self-assembles into much thinner fibrils, that form a more inhomogeneous and softer network, with a fourfold reduction in elastic modulus when compared to H[Formula: see text]O. Combining spectroscopic measurements with atomistic simulations, we show that collagen in D[Formula: see text]O is less hydrated than in H[Formula: see text]O. This partial dehydration lowers the enthalpic penalty for water removal and reorganization at the collagen-water interface, increasing the self-assembly rate and the number of nucleation centers, leading to thinner fibrils and a softer network. Coarse-grained simulations show that the acceleration in the initial nucleation rate can be reproduced by the enhancement of electrostatic interactions. These results show that water acts as a mediator between collagen monomers, by modulating their interactions so as to optimize the assembly process and, thus, the final network properties. We believe that isotopically modulating the hydration of proteins can be a valuable method to investigate the role of water in protein structural dynamics and protein self-assembly.

Resolving Multi-Asperity Contacts at the Nanoscale through Super-Resolution Fluorescence Imaging.

Contact mechanics, spanning nanometer to tectonic scales, faces long-standing challenges arising from multiscale random roughness, which hinders experimental validation of theories. Understanding multi-asperity rough contacts is vital for addressing catastrophic consequences of these contacts failing such as earthquakes and for diverse technological applications. To visualize such contacts, we introduce a super-resolution microscopy method utilizing spontaneous millisecond ON/OFF fluorescence blinking of contact-sensitive molecular rotor molecules immobilized on a glass coverslip. This technique achieves ∼55 nm lateral imaging resolution for rough poly(methyl methacrylate) and glass spheres on glass contacts. For soft polymer spheres due to large plastic deformation, the resolution improvement does not significantly affect the area of real contact. However, for hard glass spheres, the real contact area is found to be 2.4 times smaller than that found by diffraction-limited imaging. This study highlights, through direct visualization, the impact of material stiffness on the nanoscale structure within the area of real contact.

Visualization of the Sol-Gel Transition in Porous Networks Using Fluorescent Viscosity-Sensitive Probes.

The sol-gel transition involves the transformation of a colloidal suspension into a system-spanning, interconnected gel. This process is widely used to reinforce mechanically weakened porous artifacts, such as sculptures but the impact of the restricted geometry (porous network) on the gelation dynamics of the solution remains unclear. Here, using fluorescent viscosity-sensitive molecular rotors, confocal microscopy, and model pores, we visualize the local viscosity changes at the microscale that accompany the sol-gel transition of a methyltriethoxysilane solution into a gel network. We show that, with evaporation of the solvent, a viscosity gradient develops near the free surface, triggering the sol-gel transition inside small pores near the surface. In homogeneous porous media, this leads to skin formation, which reduces the evaporation rate. In heterogeneous porous media, a gradient in gel density develops toward the heart of the porous material, where the gel formation mainly occurs as capillary bridges within smaller pores.

Droplet Size Distribution in Emulsions.

The droplet size in emulsions is known to affect the rheological properties and plays a crucial role in many applications of emulsions. Despite its importance, the underlying mechanisms governing droplet size in emulsification remain poorly understood. We investigate the average drop size and size distribution upon emulsification with a high-shear mixer for model oil-in-water emulsions stabilized by a surfactant. The size distribution is found to be a log-normal distribution resulting from the repetitive random breakup of drops. High-shear emulsification, the usual way of making emulsions, is therefore found to be very different from turbulent emulsification given by the Kolmogorov-Hinze theory, for which power-law distributions of the drop size are expected. In agreement with this, the mean droplet size does not follow a scaling with the Reynolds number of the emulsification flow but rather a capillary number scaling based on the viscosity of the continuous phase.

Capillary Forces Lead to Pendant Crystals at the Liquid-Air Interface of Evaporating Salt Solutions.

We investigated the nucleation and growth processes of individual NaCl crystals from an evaporating salt solution that is supersaturated. We find that crystals nucleate at the liquid/vapor interface, resulting in distinct "pendant" crystals, which reach millimeter dimensions. The substantial size of the crystals induces deformation of the interface. This process and the evaporation rate, in turn, determine the final crystal shape, which features a deep central cavity. Our findings reveal that a delicate balance exists between gravity, buoyancy, and the surface tension of the liquid/vapor interface that allows the crystal to remain pendant. When the contact angle of the crystal with the meniscus reaches 90°, the crystal disconnects from the interface and falls into the solution. We quantitatively predict the critical mass at which this occurs.

Controlling Macroscopic Friction through Interfacial Siloxane Bonding.

Controlling macroscopic friction is crucial for numerous natural and industrial applications, ranging from forecasting earthquakes to miniaturizing semiconductor devices, but predicting and manipulating friction phenomena remains a challenge due to the unknown relationship between nanoscale and macroscopic friction. Here, we show experimentally that dry friction at multiasperity Si-on-Si interfaces is dominated by the formation of interfacial siloxane (Si─O─Si) bonds, the density of which can be precisely regulated by exposing plasma-cleaned silicon surfaces to dry nitrogen. Our results show how the bond density can be used to quantitatively understand and control the macroscopic friction. Our findings establish a unique connection between the molecular scale at which adhesion occurs, and the friction coefficient that is the key macroscopic parameter for industrial and natural tribology challenges.

Super-resolution Fluorescence Imaging of Recycled Polymer Blends via Hydrogen Bond-Assisted Adsorption of a Nile Red Derivative.

A key challenge in the recycling of multilayer plastic films of polyethylene and polyamide, as typically used for food packaging, is to assess and control the phase separation of the two types of polymers in the recycled material, the specifics of which determine the mechanical strength of the recycled material. However, visualizing the polyamide-in-polyethylene domains with conventional fluorescence methods or electron microscopy is challenging. We present a new approach that combines the point accumulation in nanoscale topography (PAINT) super-resolution method with a newly synthesized Nile Red probe (diOHNR) as the fluorescent label. The molecule was modified to undergo a hydrogen bond-assisted interaction with the polyamide phase in the blend due to its two additional hydroxyl groups but preserves the spectral properties of Nile Red. As a result, the localization density of the probe in the PAINT image is 13 times larger at the polyamide phase than at the polyethylene phase, enabling quantitative evaluation of the spatial polyamide/polyethylene distribution down to the nanoscale. The method achieved a spatial resolution of 18.8 nm, and we found that over half of the polyamide particles in a recycled sample were smaller than the optical diffraction limit. Being able to image the blends with nanoscopic resolution can help to optimize the composition and mechanical properties of recycled materials and thus contribute to an increased reuse of plastics.

Generation of Aerosols by Noninvasive Respiratory Support Modalities: A Systematic Review and Meta-Analysis.

Importance: Infection control guidelines have historically classified high-flow nasal oxygen and noninvasive ventilation as aerosol-generating procedures that require specialized infection prevention and control measures. Objective: To evaluate the current evidence that high-flow nasal oxygen and noninvasive ventilation are associated with pathogen-laden aerosols and aerosol generation. Data Sources: A systematic search of EMBASE and PubMed/MEDLINE up to March 15, 2023, and CINAHL and ClinicalTrials.gov up to August 1, 2023, was performed. Study Selection: Observational and (quasi-)experimental studies of patients or healthy volunteers supported with high-flow nasal oxygen or noninvasive ventilation were selected. Data Extraction and Synthesis: Three reviewers were involved in independent study screening, assessment of risk of bias, and data extraction. Data from observational studies were pooled using a random-effects model at both sample and patient levels. Sensitivity analyses were performed to assess the influence of model choice. Main Outcomes and Measures: The main outcomes were the detection of pathogens in air samples and the quantity of aerosol particles. Results: Twenty-four studies were included, of which 12 involved measurements in patients and 15 in healthy volunteers. Five observational studies on SARS-CoV-2 detection in a total of 212 air samples during high-flow nasal oxygen in 152 patients with COVID-19 were pooled for meta-analysis. There was no association between high-flow nasal oxygen and pathogen-laden aerosols (odds ratios for positive samples, 0.73 [95% CI, 0.15-3.55] at the sample level and 0.80 [95% CI, 0.14-4.59] at the patient level). Two studies assessed SARS-CoV-2 detection during noninvasive ventilation (84 air samples from 72 patients). There was no association between noninvasive ventilation and pathogen-laden aerosols (odds ratios for positive samples, 0.38 [95% CI, 0.03-4.63] at the sample level and 0.43 [95% CI, 0.01-27.12] at the patient level). None of the studies in healthy volunteers reported clinically relevant increases in aerosol particle production by high-flow nasal oxygen or noninvasive ventilation. Conclusions and Relevance: This systematic review and meta-analysis found no association between high-flow nasal oxygen or noninvasive ventilation and increased airborne pathogen detection or aerosol generation. These findings argue against classifying high-flow nasal oxygen or noninvasive ventilation as aerosol-generating procedures or differentiating infection prevention and control practices for patients receiving these modalities.

Predicting frictional aging from bulk relaxation measurements.

The coefficient of static friction between solids normally increases with the time they have remained in static contact before the measurement. This phenomenon, known as frictional aging, is at the origin of the difference between static and dynamic friction coefficients but has remained difficult to understand. It is usually attributed to a slow expansion of the area of atomic contact as the interface changes under pressure. This is however challenging to quantify as surfaces have roughness at all length scales. In addition, friction is not always proportional to the contact area. Here we show that the normalized stress relaxation of the surface asperities during frictional contact with a hard substrate is the same as that of the bulk material, regardless of the asperities' size or degree of compression. This result enables us to predict the frictional aging of rough interfaces based on the bulk material properties of two typical polymers: polypropylene and polytetrafluoroethylene.

Low energy nebulization preserves integrity of SARS-CoV-2 mRNA vaccines for respiratory delivery.

Nebulization of mRNA therapeutics can be used to directly target the respiratory tract. A promising prospect is that mucosal administration of lipid nanoparticle (LNP)-based mRNA vaccines may lead to a more efficient protection against respiratory viruses. However, the nebulization process can rupture the LNP vehicles and degrade the mRNA molecules inside. Here we present a novel nebulization method able to preserve substantially the integrity of vaccines, as tested with two SARS-CoV-2 mRNA vaccines. We compare the new method with well-known nebulization methods used for medical respiratory applications. We find that a lower energy level in generating LNP droplets using the new nebulization method helps safeguard the integrity of the LNP and vaccine. By comparing nebulization techniques with different energy dissipation levels we find that LNPs and mRNAs can be kept largely intact if the energy dissipation remains below a threshold value, for LNP integrity 5-10 J/g and for mRNA integrity 10-20 J/g for both vaccines.

Quantitative Understanding of the Onset of Dense Granular Flows.

The question of when and how dense granular materials start to flow under stress, despite many industrial and geophysical applications, remains largely unresolved. We develop and test a simple equation for the onset of quasistatic flows of granular materials which is based on the frictional aging of the granular packing. The result is a nonmonotonic stress-strain relation which-akin to classical friction-is independent of the shear rate. This relation suffices to understand the quasistatic deformations of aging granular media, and its solid-to-liquid transition. Our results also elucidate the (flow) history dependence of the mechanical properties, and the sensitivity to the initial preparation of granular media.

Surface-Mediated Molecular Transport of a Lipophilic Fluorescent Probe in Polydisperse Oil-in-Water Emulsions.

Emulsions often act as carriers for water-insoluble solutes that are delivered to a specific target. The molecular transport of solutes in emulsions can be facilitated by surfactants and is often limited by diffusion through the continuous phase. We here investigate this transport on a molecular scale by using a lipophilic molecular rotor as a proxy for solutes. Using fluorescence lifetime microscopy we track the transport of these molecules from the continuous phase toward the dispersed phase in polydisperse oil-in-water emulsions. We show that this transport comprises two time scales, which vary significantly with droplet size and surfactant concentration, and, depending on the type of surfactant used, can be limited either by transport across the oil-water interface or by diffusion through the continuous phase. By studying the time-resolved fluorescence of the fluorophore, accompanied by molecular dynamics simulations, we demonstrate how the rate of transport observed on a macroscopic scale can be explained in terms of the local environment that the probe molecules are exposed to.