Linking structural and rheological memory in disordered soft materials.

Linking the macroscopic flow properties and nanoscopic structure is a fundamental challenge to understanding, predicting, and designing disordered soft materials. Under small stresses, these materials are soft solids, while larger loads can lead to yielding and the acquisition of plastic strain, which adds complexity to the task. In this work, we connect the transient structure and rheological memory of a colloidal gel under cyclic shearing across a range of amplitudes a generalized memory function using rheo-X-ray photon correlation spectroscopy (rheo-XPCS).

Spatial Photo-Patterning of Nematic Liquid Crystal Pretilt and its Application in Fabricating Flat Gradient-Index Lenses.

Liquid crystals offer a dynamic platform for developing advanced photonics and soft actuation systems due to their unique and facile tunability and reconfigurability. Achieving precise spatial patterning of the liquid crystal alignment is critical to developing electro-optical devices, programmable origami, directed colloidal assembly, and controlling active matter. Here, a simple method is demonstrated to achieve continuous 3D control of the directions of liquid crystal mesogens using a two-step photo-exposure process.

Tunable three-dimensional architecture of nematic disclination lines.

Disclination lines play a key role in many physical processes, from the fracture of materials to the formation of the early universe. Achieving versatile control over disclinations is key to developing novel electro-optical devices, programmable origami, directed colloidal assembly, and controlling active matter. Here, we introduce a theoretical framework to tailor three-dimensional disclination architecture in nematic liquid crystals experimentally.

Investigation of the yielding transition in concentrated colloidal systems via rheo-XPCS.

We probe the microstructural yielding dynamics of a concentrated colloidal system by performing creep/recovery tests with simultaneous collection of coherent scattering data via X-ray Photon Correlation Spectroscopy (XPCS). This combination of rheology and scattering allows for time-resolved observations of the microstructural dynamics as yielding occurs, which can be linked back to the applied rheological deformation to form structure-property relations. Under sufficiently small applied creep stresses, examination of the correlation in the flow direction reveals that the scattering response recorrelates with its predeformed state, indicating nearly complete microstructural recovery, and the dynamics of the system under these conditions slows considerably.

Memory in aging colloidal gels with time-varying attraction.

We report a combined rheology, x-ray photon correlation spectroscopy, and modeling study of gel formation and aging in suspensions of nanocolloidal spheres with volume fractions of 0.20 and 0.43 and with a short-range attraction whose strength is tuned by changing temperature.

Microscopic dynamics underlying the stress relaxation of arrested soft materials.

Arrested soft materials such as gels and glasses exhibit a slow stress relaxation with a broad distribution of relaxation times in response to linear mechanical perturbations. Although this macroscopic stress relaxation is an essential feature in the application of arrested systems as structural materials, consumer products, foods, and biological materials, the microscopic origins of this relaxation remain poorly understood. Here, we elucidate the microscopic dynamics underlying the stress relaxation of such arrested soft materials under both quiescent and mechanically perturbed conditions through X-ray photon correlation spectroscopy.

Dynamic and mechanical evolution of an oil-water interface during bacterial biofilm formation.

We present an experimental study combining particle tracking, active microrheology, and differential dynamic microscopy (DDM) to investigate the dynamics and rheology of an oil-water interface during biofilm formation by the bacteria PA14. The interface transitions from an active fluid dominated by the swimming motion of adsorbed bacteria at early age to an active viscoelastic system at late ages when the biofilm is established. The microrheology measurements using microscale magnetic rods indicate that the biofilm behaves as a viscoelastic solid at late age.

Interfacial behaviour of β-lactoglobulin aggregates at the oil-water interface studied using particle tracking and dilatational rheology.

During processing, proteins are easily self-assembled into different aggregates, such as nanoparticles and fibrils. Protein aggregates exhibit a strong interfacial activity due to their morphologies and functional groups on the surface. Their interfacial structure and rheological properties at the oil-water interface have a significant effect on the stability and fat digestion of emulsions in food.

Microscopic ergodicity breaking governs the emergence and evolution of elasticity in glass-forming nanoclay suspensions.

We report a study combining x-ray photon correlation spectroscopy (XPCS) with in situ rheology to investigate the microscopic dynamics and mechanical properties of aqueous suspensions of the synthetic hectorite clay Laponite, which is composed of charged, nanometer-scale, disk-shaped particles. The suspensions, with particle concentrations ranging from 3.25 to 3.

Driven topological transitions in active nematic films.

The topological properties of many materials are central to their behavior. In intrinsically out-of-equilibrium active materials, the dynamics of topological defects can be particularly important. In this paper, local manipulation of the order, dynamics, and topological properties of microtubule-based active nematic films is demonstrated in a joint experimental and simulation study.

In situ nanomechanical properties of natural oil bodies studied using atomic force microscopy.

Natural oil bodies (OBs) from plant organs represent an important category of functional ingredients and materials in a variety of industrial sectors. Their applications are closely related to the membrane mechanical properties on a single droplet level, which remain difficult to determine. In this research, the mechanical properties of the membranes of OBs from soybean, sesame, and peanut were investigated in-situ by atomic force microscopy (AFM).

Author Correction: Films of Bacteria at Interfaces (FBI): Remodeling of Fluid Interfaces by Pseudomonas aeruginosa.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Evolution of structure and dynamics of thermo-reversible nanoparticle gels-A combined XPCS and rheology study.

A combined X-ray photon correlation spectroscopy and rheology study is carried out to capture the evolution of structure, fast particle-scale dynamics, and moduli (elastic and loss) at early times of gel formation near the fluid-gel boundary of a suspension of nanoparticles. The system is comprised of moderately concentrated suspensions of octadecyl silica in decalin (ϕ = 0.2) undergoing thermoreversible gelation.

Phase-dependent shear-induced order of nanorods in isotropic and nematic wormlike micelle solutions.

Small angle X-ray scattering with in situ shear was employed to study the assembly and ordering of dispersions of gold nanorods within wormlike micelle solutions formed by the surfactant cetylpyridinium chloride (CPyCl) and counter-ion sodium salicylate (NaSal). Above a threshold CPyCl concentration but below the isotropic-to-nematic transition of the micelles, the nanorods self-assembled under quiescent conditions into isotropically oriented domains with hexagonal order. Under steady shear at rates between 0.

Cargo carrying bacteria at interfaces.

The displacements of ensembles of colloids at the interface between oil and suspensions of the bacterium Pseudomonas aeruginosa PA14ΔpelA indicate enhanced colloid mobilities and apparently diffusive motion driven by interactions with the bacteria. However, inspection of individual trajectories of ∼500 particles reveals prolonged, directed displacements inconsistent with purely hydrodynamic interactions between swimming bacteria and colloids. Analysis of the properties of colloid paths indicates trajectories can be sorted into four distinct categories, including diffusive, persistent, curly, and mixed trajectory types.

Enhanced gel formation in binary mixtures of nanocolloids with short-range attraction.

Colloidal suspensions transform between fluid and disordered solid states as parameters such as the colloid volume fraction and the strength and nature of the colloidal interactions are varied. Seemingly subtle changes in the characteristics of the colloids can markedly alter the mechanical rigidity and flow behavior of these soft composite materials. This sensitivity creates both a scientific challenge and an opportunity for designing suspensions for specific applications.

Correction: Films of bacteria at interfaces: three stages of behaviour.

Correction for 'Films of bacteria at interfaces: three stages of behaviour' by Liana Vaccari et al., Soft Matter, 2015, 11, 6062-6074.

Films of Bacteria at Interfaces (FBI): Remodeling of Fluid Interfaces by Pseudomonas aeruginosa.

Bacteria at fluid interfaces endure physical and chemical stresses unique to these highly asymmetric environments. The responses of Pseudomonas aeruginosa PAO1 and PA14 to a hexadecane-water interface are compared. PAO1 cells form elastic films of bacteria, excreted polysaccharides and proteins, whereas PA14 cells move actively without forming an elastic film.

Dynamic Scaling of Colloidal Gel Formation at Intermediate Concentrations.

We have examined the formation and dissolution of gels composed of intermediate volume-fraction nanoparticles with temperature-dependent short-range attractions using small-angle x-ray scattering, x-ray photon correlation spectroscopy, and rheology to obtain nanoscale and macroscale sensitivity to structure and dynamics. Gel formation after temperature quenches to the vicinity of the rheologically determined gel temperature, T_{gel}, was characterized via the slowdown of dynamics and changes in microstructure observed in the intensity autocorrelation functions and structure factor, respectively, as a function of quench depth (ΔT=T_{quench}-T_{gel}), wave vector, and formation time t_{f}. We find the wave-vector-dependent dynamics, microstructure, and rheology at a particular ΔT and t_{f} map to those at other ΔTs and t_{f}s via an effective scaling temperature, T_{s}.

Colloidal transport within nematic liquid crystals with arrays of obstacles.

We have investigated the gravity-driven transport of spherical colloids suspended in the nematic liquid crystal 4-cyano-4'-pentylbiphenyl (5CB) within microfluidic arrays of cylindrical obstacles arranged in a square lattice. Homeotropic anchoring at the surfaces of the obstacles created periodic director-field patterns that strongly influenced the motion of the colloids, whose surfaces had planar anchoring. When the gravitational force was oriented parallel to a principal axis of the lattice, the particles moved along channels between columns of obstacles and displayed pronounced modulations in their velocity.

Films of bacteria at interfaces.

Bacteria are often discussed as active colloids, self-propelled organisms whose collective motion can be studied in the context of non-equilibrium statistical mechanics. In such studies, the behavior of bacteria confined to interfaces or in the proximity of an interface plays an important role. For instance, many studies have probed collective behavior of bacteria in quasi two-dimensional systems such as soap films.

Photoactivatable fluorescent probes reveal heterogeneous nanoparticle permeation through biological gels at multiple scales.

Diffusion through biological gels is crucial for effective drug delivery using nanoparticles. Here, we demonstrate a new method to measure diffusivity over a large range of length scales - from tens of nanometers to tens of micrometers - using photoactivatable fluorescent nanoparticle probes. We have applied this method to investigate the length-scale dependent mobility of nanoparticles in fibrin gels and in sputum from patients with cystic fibrosis (CF).

Exploring the relationship between nanoscale dynamics and macroscopic rheology in natural polymer gums.

We report a study connecting the nanoscale and macroscale structure and dynamics of Acacia mearnsii gum as probed by small-angle X-ray scattering (SAXS), X-ray photon correlation spectroscopy (XPCS) and rheology. Acacia gum, in general, is a complex polysaccharide used extensively in industry. Over the analyzed concentration range (15 to 30 wt%) the A.

Films of bacteria at interfaces: three stages of behaviour.

We report an investigation of the formation of films by bacteria at an oil-water interface using a combination of particle tracking and pendant drop elastometry. The films display a remarkably varied series of dynamical and mechanical properties as they evolve over the course of minutes to hours following the creation of an initially pristine interface. At the earliest stage of formation, which we interrogate using dispersions of colloidal probes, the interface is populated with motile bacteria.