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Colloidal gels formed by arrested phase separation are found widely in agriculture, biotechnology, and advanced manufacturing; yet, the emergence of elasticity and the nature of the arrested state in these abundant materials remains unresolved. Here, the quantitative agreement between integrated experimental, computational, and graph theoretic approaches are used to understand the arrested state and the origins of the gel elastic response. The micro-structural source of elasticity is identified by the l -balanced graph partition of the gels into minimally interconnected clusters that act as rigid, load bearing units. The number density of cluster-cluster connections grows with increasing attraction, and explains the emergence of elasticity in the network through the classic Cauchy-Born theory. Clusters are amorphous and iso-static. The internal cluster concentration maps onto the known attractive glass line of sticky colloids at low attraction strengths and extends it to higher strengths and lower particle volume fractions. Colloidal gels are typically composed of solid particles dispersed in a liquid, which show some peculiar mechanic properties but their origins remain largely unsolved. Here, Whitaker et al. show that the elasticity formed via arrested phase separation arises from the packing of glassy clusters in gels.

Measuring polymer surface dynamics remains a formidable challenge of critical importance to applications ranging from pressure-sensitive adhesives to nanopatterning, where interfacial mobility is key to performance. Here, we introduce a methodology of Brillouin light spectroscopy to reveal polymer surface mobility via nanoparticle vibrations. By measuring the temperature-dependent vibrational modes of polystyrene nanoparticles, we identify the glass-transition temperature and calculate the elastic modulus of individual nanoparticles as a function of particle size and chemistry. Evidence of surface mobility is inferred from the first observation of a softening temperature, where the temperature dependence of the fundamental vibrational frequency of the nanoparticles reverses slope below the glass-transition temperature. Beyond the fundamental vibrational modes given by the shape and elasticity of the nanoparticles, another mode, termed the interaction-induced mode, was found to be related to the active particle–particle adhesion and dependent on the thermal behavior of nanoparticles. Measuring polymer surface dynamics is a challenge of importance to applications ranging from pressure-sensitive adhesives to nanopatterning. Here, the authors introduce a methodology of Brillouin light spectroscopy to reveal polymer surface mobility via nanoparticle vibrations.

The ageing behaviour of dense suspensions or pastes at rest is almost exclusively attributed to structural dynamics. Here, we identify another ageing process, contact-controlled ageing, consisting of the progressive stiffening of solid–solid contacts of an arrested colloidal suspension. By combining rheometry, confocal microscopy and particle-scale mechanical tests using laser tweezers, we demonstrate that this process governs the shear-modulus ageing of dense aqueous silica and polymer latex suspensions at moderate ionic strengths. We further show that contact-controlled ageing becomes relevant as soon as Coulombic interactions are sufficiently screened out that the formation of solid–solid contacts is not limited by activation barriers. Given that this condition only requires moderate ion concentrations, contact-controlled ageing should be generic in a wide class of materials, such as cements, soils or three-dimensional inks, thus questioning our understanding of ageing dynamics in these systems. The progressive stiffening of the solid–solid contacts that freeze dense colloidal suspensions are shown to cause the macroscopic ageing of such materials.

Polarizable colloids are expected to form crystalline equilibrium phases when exposed to a steady, uniform field. However, when colloids become localized this field-induced phase transition arrests and the suspension persists indefinitely as a kinetically trapped, percolated structure. We anneal such gels formed from magneto-rheological fluids by toggling the field strength at varied frequencies. This processing allows the arrested structure to relax periodically to equilibrium—colloid-rich, cylindrical columns. Two distinct growth regimes are observed: one in which particle domains ripen through diffusive relaxation of the gel, and the other where the system-spanning structure collapses and columnar domains coalesce apparently through field-driven interactions. There is a stark boundary as a function of magnetic field strength and toggle frequency distinguishing the two regimes. These results demonstrate how kinetic barriers to a colloidal phase transition are subverted through measured, periodic variation of driving forces. Such directed assembly may be harnessed to create unique materials from dispersions of colloids.

Janus ellipsoids self-assemble into self-limiting fibres that can be reversibly actuated by applying an electric field. Michael Solomon et al show that assemblies made of ellipsidal colloids held together by attractive patches form ordered cluster and brillar phases, and that the brillar assemblies of ellipsoids reversibly stretch and contract in an electric field.

Soft materials are usually defined as materials made of mesoscopic entities, often self-organised, sensitive to thermal fluctuations and to weak perturbations. Archetypal examples are colloids, polymers, amphiphiles, liquid crystals, foams. The importance of soft materials in everyday commodity products, as well as in technological applications, is enormous, and controlling or improving their properties is the focus of many efforts. From a fundamental perspective, the possibility of manipulating soft material properties, by tuning interactions between constituents and by applying external perturbations, gives rise to an almost unlimited variety in physical properties. Together with the relative ease to observe and characterise them, this renders soft matter systems powerful model systems to investigate statistical physics phenomena, many of them relevant as well to hard condensed matter systems. Understanding the emerging properties from mesoscale constituents still poses enormous challenges, which have stimulated a wealth of new experimental approaches, including the synthesis of new systems with, e.g. tailored self-assembling properties, or novel experimental techniques in imaging, scattering or rheology. Theoretical and numerical methods, and coarse-grained models, have become central to predict physical properties of soft materials, while computational approaches that also use machine learning tools are playing a progressively major role in many investigations. This Roadmap intends to give a broad overview of recent and possible future activities in the field of soft materials, with experts covering various developments and challenges in material synthesis and characterisation, instrumental, simulation and theoretical methods as well as general concepts.

A method is presented to estimate the static error 𝜖 in a multiple particle tracking microrheology experiment. This in situ estimate of 𝜖 is measured under the same conditions of the material under test, and without any additional experiments. The correction of the mean-squared displacement by the in situ method is potentially more reliable than methods that rely on characterizing 𝜖 in a separate gel sample. With the true mean-squared displacements accessible at short lag times, experimental artifacts introduced by static error can be distinguished from true rheological properties, even in highly viscous (>10,000 mPa⋅s) samples.

A tracking method and statistical analysis is introduced to quantify the mixing of moving droplets in the Lagrangian reference frame. Aqueous microrheology samples are produced as droplets in immiscible oil using a microfluidic T-junction. Samples from initially unmixed streams of the same viscosity-fluids (water/water) or different viscosity-fluids (water/glycerin solution) are dyed with different colors to visualize their internal motions and to quantify the extent of their mixing as a function of the age in the channel. The homogeneity of the material distribution in the drop is quantified by computing skewness of pixel intensity profiles or Shannon entropy index. Such analysis is important to ensure that samples are uniformly mixed for high-throughput rheological measurements using microrheology. Samples with a high viscosity ratio mix more rapidly than those with the same viscosities and the mixing length in traversing drops in the microchannel decays exponentially with traveling displacement until the drop reaches a diffusion limit.

Dense colloidal suspensions are processed in a wide variety of industries. Challenges for pumping suspensions and slurries at high concentrations include shear thickening and dilation, which can have deleterious consequences. These systems are shear sensitive close to the jamming point, meaning that a significant increase in high shear viscosity can be observed with just a few percent change in volume fractions. Therefore, accurate and rapid determination of the jamming point can greatly aid formulation. Typically, conventional rheometry identifies the jamming point by a time-consuming process, whereby multiple flow curves of suspensions of different volume fraction are measured and extrapolated to the volume fraction where the viscosity diverges. We present an alternative approach for rapid, one-step, experimental determination of the jamming point for aqueous suspensions. The procedure monitors the shear stress under constant shear stress or shear rate as the sample is dewatered using immobilization cell rheometry, until the viscosity diverges. The method is validated by comparing the results of this work with conventional rheometry for a model suspension. Then it is applied to examine the effect of grafting a short-chain polymer to particles, comprising an industrial suspension of silica-coated titania. Polymeric coating of the particles increases the jamming concentration and mitigates shear thickening, qualitatively consistent with predictions from simulations. Graphical Abstract A new method is designed to extract the jamming point of a suspension. The procedure monitors the effective viscosity under prescribed shear conditions as the suspension is dewatered using immobilization cell rheometry. The geometry moves down to accommodate solvent evaporation, until the viscosity diverges, and the jamming point is reached.