We present a dynamic light scattering setup to probe, with time and space resolution, the microscopic dynamics of soft matter systems confined within millimeter-sized spherical drops. By using an ad hoc optical layout, we tackle the challenges raised by refraction effects due to the unconventional shape of the samples. We first validate the setup by investigating the dynamics of a suspension of Brownian particles. The dynamics measured at different positions in the drop, and hence different scattering angles, are found to be in excellent agreement with those obtained for the same sample in a conventional light scattering setup. We then demonstrate the setup capabilities by investigating a bead made of a polymer hydrogel undergoing swelling. The gel microscopic dynamics exhibit a space dependence that strongly varies with time elapsed since the beginning of swelling. Initially, the dynamics in the periphery of the bead are much faster than in the core, indicative of nonuniform swelling. As the swelling proceeds, the dynamics slow down and become more spatially homogeneous. By comparing the experimental results to numerical and analytical calculations for the dynamics of a homogeneous, purely elastic sphere undergoing swelling, we establish that the mean square displacement of the gel strands deviates from the affine motion inferred from the macroscopic deformation, evolving from fast diffusivelike dynamics at the onset of swelling to slower, yet supradiffusive, rearrangements at later stages.

Tough soft materials such as multiple network elastomers (MNE) or filled elastomers are typically stretchable and include significant energy dissipation mechanisms that prevent or delay crack growth. Yet most studies and fracture models focus on steady-state propagation and damage is assumed to be decoupled from the local stress and strain fields near the crack tip. We report an in situ spatial-temporally resolved 3D measurement of molecular damage in mechanophore-labeled MNE just before a crack propagates. This technique, complemented by digital image correlation, allows us to compare the spatial distribution of both damage and deformation in single network (SN) elastomers and in MNE. Compared to SN, MNE have a wide-spread damage in front of the crack and, surprisingly, delocalize strain concentration. A continuum model, where damage distribution is fully coupled to the crack tip fields, is proposed to explain these results. Additional measurements of time-dependent molecular damage during fixed grips relaxation in the presence of a crack reveal that the less localized damage distribution delays fracture initiation. The observations and exploratory modeling reveal the dynamic fracture mechanism of MNE, providing guidance for rational design of high-performance tough elastomers.

The study delves into the adsorption of sunflower proteins at the air/water interface using specular X-ray reflection. The research involved fitting models of the protein films to the reflectivity data, resulting in detailed images of the X-ray scattering length density profiles perpendicular to the air/water interface. The sunflower protein isolate that is examined consists of multiple components, and the study proposes a transition from a 1-slab model to a 4-slab model to represent the changing layer structure over time. This transition is significant as it reflects the increasing complexity of the protein film as more proteins adsorb at the interface. Initially, sunflower proteins form a monolayer at the air/water boundary, consisting of a protein-rich, hydrophobic portion closest to the interface and a more diffuse, hydrophilic portion extending into the bulk aqueous phase. The structural changes at the interface over time depend on the bulk protein concentration in the solution. For solutions at relatively low concentrations (C ≤ 0.5 g/L), a lower amount of adsorption results in a larger, more extensive interface area for each species and a thinner protein adsorption layer. The overall thickness of a saturated monolayer is approximately 100 Å, which is close to the maximum dimension of sunflower globulins, with the thickness of the corresponding hydrophobic portion being about 20 Å. For solutions at relatively high concentrations (C ≥ 1.0 g/L), even after forming a saturated monolayer, structural evolution continues within the experimental time frame, occurring on both hydrophilic and hydrophobic sides. Additional proteins from the bulk diffuse toward the interface, forming an extra layer in the water phase and causing an increase in the overall thickness. Furthermore, a distinct sublayer develops next to the air phase, indicating a further structuration of the hydrophobic portion.

Foams age as gas diffuses from smaller bubbles to larger ones. This results in an increase of the average bubble size, which leads to a modification of the foam rheology and overall stability. This is why understanding coarsening is crucial for the creation of aerated materials. The coarsening rate is affected by various mechanisms, which are impacted by geometry (bubble size and bubble size distribution), liquid fraction, air solubility in the liquid phase, permeability of the interfaces, mechanical properties of the liquid phase and of the interfaces. In many real systems changing a single parameter will impact several mechanisms. In this work, we use a two -bubble experiment to isolate and explore the impact of bulk and surface viscosity on the rate of bubble coarsening. The experimental set-up allows us to decouple the impact of viscous dissipation from the rate of gas diffusion. We build a model in which the gas transfer is driven by Laplace pressure differences and hindered by viscous stresses. We need to take into account gravitational stresses, and dissipation in the connections, with which our model is fully predictive of the experimental data.

Gemini surfactants are ideal systems to study a wide range of rheological behaviours in soft matter, showing fascinating analogies with living polymers and polyelectrolytes. By only changing the concentration, the shear viscosity can vary by 7 orders of magnitude in the bulk when transitioning through the semidilute regime. In order to elucidate on the intrinsic shear viscosity profile at the interface in soft matter systems manifesting various concentration regimes and morphological transitions, we performed microrheology and adsorption experiments under a wide range of experimental conditions. The surface shear viscosity has been characterized by passive microrheology, tracking Brownian particles trapped at the air-solution interface, under particle wetting conditions precisely characterized by interferometry. We observe that a steep increase in bulk shear viscosity as a function of the concentration does not translate at the interface, which may show a negative surface shear viscosity. By comparing macrorheology and microrheology, we measure significant differences both at the interface and in the bulk in the semidilute regime, where wormlike micelles start to entangle. The disparity in rheological measurements can be attributed to notable depletion effects near both the air-solution and particle-solution interfaces.