Soft Matter最新文献

This paper presents a systematic investigation of the crystalline nucleation, micellization, two-dimensional (2D) growth of polyethylene-b-hyperbranched polyglycidol (PE-b-hbPG) copolymers in solutions during cooling and isothermal crystallization. As a result, lozenge-shaped monolayer or multilayer lamellar crystals were prepared by optimizing the “self-nucleation” conditions. The effect of crystallization temperatures (T_c), critical micelle temperature (CMT), selective solvents, and the topology of block copolymers (BCPs) on the growth of 2D lozenge-shaped crystals is extensively explored using TEM, AFM and in situ DLS techniques. The results demonstrate that the formation of a perfect lozenge-shaped monolayer crystal is contingent upon the relationship between CMT and T_c of the BCPs (CMT < T_c), as well as the isothermal crystallization temperature T_iso (CMT < T_iso < T_c). This significant finding provides a feasibility programme for the preparation of 2D lamellar crystals using the “self-nucleation” approach from an alternative viewpoint of the corona topology.

We study poly-crystalline spherical drops of an aqueous suspension of highly charged colloidal spheres exposed to a colloid-free aqueous environment. Crystal contours were obtained from standard optical imaging. The crystal spheres first expand to nearly four times their initial volume before slowly shrinking due to dilution-induced melting. Exploiting coherent multiple-scattering by (110) Bragg reflecting crystals, time-dependent density profiles were recorded within the drop interior. These show a continuously flattening radial density gradient and a decreasing central density. Expansion curves and density profiles are qualitatively consistent with theoretical expectations based on dynamical density functional theory for the expansion of a spherical crystallite made of charged Brownian spheres. We anticipate that our study opens novel experimental access to density determination in turbid crystals.

The mussel thread-plaque system exhibits strong adhesion and high deformability, allowing it to adhere to various surfaces. While the microstructure of plaques has been thoroughly studied, the effect of their unique porous structure on the high deformability remains unclear. This study first investigated the porous structure of mussel plaque cores using scanning electron microscopy (SEM). Two-dimensional (2D) porous representative volume elements (RVEs) with scaled distribution parameters were generated, and the calibrated phase-field modelling method was applied to analyse the effect of the pore distribution and multi-scale porous structure on the failure mechanism of porous RVEs. The SEM analysis revealed that large-scale pores exhibited a lognormal size distribution and a uniform spatial distribution. Simulations showed that increasing the normalised mean radius value (ū) of the large-scale pore distribution can statistically lead to a decreasing trend in final failure strain, strength and strain energy density but cannot solely determine their values. The interaction between pores can lead to two different failure modes under the same pore distribution: progressive failure mode and sudden failure mode. Additionally, the hierarchical structure of multi-scale porous RVEs can further increase the final failure strain by 40–60% compared to single-scale porous RVEs by reducing stiffness, highlighting the hierarchical structure could be another key factor contributing to the high deformability. These findings deepen our understanding of how the pore distribution and multi-scale porous structure in mussel plaques contribute to their high deformability and affect other mechanical properties, providing valuable insights for the future design of highly deformable biomimetic materials.

By introducing geometry-based phoresis kernels, we establish a direct connection between the translational and rotational velocities of a phoretic sphere and the distributions of the driving fields or fluxes. The kernels quantify the local contribution of the field or flux to the particle dynamics. The field kernels for both passive and active particles share the same functional form, depending on the position-dependent surface phoretic mobility. For uniform phoretic mobility, the translational field kernel is proportional to the surface normal vector, while the rotational field kernel is zero; thus, a phoretic sphere with uniform phoretic mobility does not rotate. As case studies, we discuss examples of a self-phoretic axisymmetric particle influenced by a globally-driven field gradient, a general scenario for axisymmetric self-phoretic particle and two of its special cases, and a non-axisymmetric active particle.

Deep learning-based optical flow (DLOF) extracts features in adjacent video frames with deep convolutional neural networks. It uses those features to estimate the inter-frame motions of objects. We evaluate the ability of optical flow to quantify the spontaneous flows of microtubule (MT)-based active nematics under different labeling conditions, and compare its performance to particle image velocimetry (PIV). We obtain flow velocity ground truths either by performing semi-automated particle tracking on samples with sparsely labeled filaments, or from passive tracer beads. DLOF produces more accurate velocity fields than PIV for densely labeled samples. PIV cannot reliably distinguish contrast variations at high densities, particularly along the nematic director. DLOF overcomes this limitation. For sparsely labeled samples, DLOF and PIV produce comparable results, but DLOF gives higher-resolution fields. Our work establishes DLOF as a versatile tool for measuring fluid flows in a broad class of active, soft, and biophysical systems.

Filamentous viruses like influenza and torovirus often display systematic bends and arcs of mysterious physical origin. We propose that such viruses undergo an instability from a cylindrically symmetric to a toroidally curved state. This “toro-elastic” state emerges via spontaneous symmetry breaking under prestress due to short range spike protein interactions magnified by surface topography. Once surface stresses are sufficiently large, the filament buckles and the curved state constitutes a soft mode that can potentially propagate through the filament's material frame around a Mexican-hat-type potential. In the mucus of our airways, which constitutes a soft, porous 3D network, glycan chains are omnipresent and influenza's spike proteins are known to efficiently bind and cut them. We next show that such a non-equilibrium enzymatic reaction can induce spontaneous rotation of the curved state, leading to a whole body reshaping propulsion similar to – but different from – eukaryotic flagella and spirochetes.

We present a comprehensive investigation combining numerical simulations with experimental validation, focusing on the creeping flow behavior of a shear-banding, viscoelastic wormlike micellar (WLM) solution over concavities with various depths (D) and lengths (L). The fluid is modeled using the diffusive Giesekus model, with model parameters set to quantitatively describe the shear rheology of a 100 : 60 mM cetylpyridinium chloride:sodium salicylate aqueous WLM solution used for the experimental validation. We observe a transition from “cavity flow” to “expansion–contraction flow” as the length L exceeds the sum of depth D and channel width W. This transition is manifested by a change of vortical structures within the concavity. For L ≤ D + W, “cavity flow” is characterized by large scale recirculations spanning the concavity length. For L > D + W, the recirculations observed in “expansion–contraction flow” are confined to the salient corners downstream of the expansion plane and upstream of the contraction plane. Using the numerical dataset, we construct phase diagrams in L–D at various fixed Weissenberg numbers Wi, characterizing the transitions and describing the evolution of vortical structures influenced by viscoelastic effects.

Colloids dispersed in nematic liquid crystals form topological composites in which colloid-associated defects mediate interactions while adhering to fundamental topological constraints. Better realising the promise of such materials requires numerical methods that model nematic inclusions in dynamic and complex scenarios. We employ a mesoscale approach for simulating colloids as mobile surfaces embedded in a fluctuating nematohydrodynamic medium to study the kinetics of colloidal entanglement. In addition to reproducing far-field interactions, topological properties of disclination loops are resolved to reveal their metastable states and topological transitions during relaxation towards ground state. The intrinsic hydrodynamic fluctuations distinguish formerly unexplored far-from-equilibrium disclination states, including configurations with localised positive winding profiles. The adaptability and precision of this numerical approach offers promising avenues for studying the dynamics of colloids and topological defects in designed and out-of-equilibrium situations.

The strength of interparticle interactions in a granular system controls how a collection of insulating particles flow, cohere and fragment. Forces due to electrostatic charging, particularly in free-fall or low gravity environments, can dominate the static and dynamic interactions with important implications for understanding natural and industrial processes. Here we show that shaking of homogeneous, spherical particles can result in a non-uniform surface charge distribution. The measured dipole moment and torque for each particle are found to be strongly correlated. However, our model shows that to predict the torque and force requires one to consider the full surface charge distribution. This overlooked torque is not only significant, but would amplify attractive interactions through particle reorientation.

Understanding and control of the effective interaction between nanoscale building blocks (colloids or nanoparticles) dispersed in a solvent is an important prerequisite for the development of bottom-up design strategies for soft functional materials. Here, we have employed all-atom molecular dynamics simulations to investigate the impact of polymer grafting on the solvent-mediated effective interaction between the silica nanoparticles (Si-NPs) in water, and in turn, on its bulk structural and thermodynamic properties. We found that the nature of the short grafting polymers [characterized by their interaction with water (hydrophobicity or hydrophilicity) and molecular weight] has a profound effect on the range and strength of the effective interaction between the Si-NPs. The hydrophobic polymer [such as polyethylene (PE)]-grafting of Si-NP gives rise to a more attractive interaction between the Si-NPs compared to the hydrophilic polymer [such as polyethylene glycol (PEG)] and non-grafted cases. This study further provides fundamental insights into the molecular origin of the observed behavior of the effective pair interactions between the grafted Si-NPs. For PE-grafted Si-NPs, the confined water (water inside the cavity formed by a pair of Si-NPs) undergoes a partial dewetting transition on approaching below a critical inter-particle separation leading to a stronger attractive interaction. Furthermore, we report that the effective attraction between the PE-grafted Si-NPs can be reliably controlled by changing the grafting PE density. We have also investigated the bulk structural and thermodynamic behavior of the coarse-grained Si-NP system where the particles interact via effective interaction in the absence of water. We believe that the insights gained from this work are important prerequisites for formulating rational bottom-up design strategies for functional materials where nano- (or, colloidal) particles are the building blocks.