We classify native and chemically modified red blood cells with an AI based video classifier. Using TensorFlow video analysis enables us to capture not only the morphology of the cell but also the trajectories of motion of individual red blood cells and their dynamics. We chemically modify cells in three different ways to model different pathological conditions and obtain classification accuracies for all three classification tasks of more than 90% between native and modified cells. Unlike standard cytometers that are based on immunophenotyping our microfluidic cytometer allows to rapidly categorize cells without any fluorescence labels simply by analysing the shape and flow of red blood cells.

Oak powdery mildew, caused by the biotrophic fungus Erysiphe alphitoides, is a prevalent disease affecting oak trees, such as English oak (Quercus robur). While mature oak populations are generally less susceptible to this disease, it can endanger young oak seedlings and new leaves on mature trees. Although disruptions of photosynthate and carbohydrate translocation have been observed, accurately detecting and understanding the specific biomolecular interactions between the fungus and the leaves of oak trees is currently lacking. Herein, via hybrid Raman spectroscopy combined with an advanced artificial neural network algorithm, the underpinning biomolecular interactions between biological soft matter, i.e., Quercus robur leaves and Erysiphe alphitoides, are investigated and profiled, generating a spectral library and shedding light on the changes induced by fungal infection and the tree's defence response. The adaxial surfaces of oak leaves are categorised based on either the presence or absence of Erysiphe alphitoides mildew and further distinguishing between covered or not covered infected leaf tissues, yielding three disease classes including healthy controls, non-mildew covered and mildew-covered. By analysing spectral changes between each disease category per tissue type, we identified important biomolecular interactions including disruption of chlorophyll in the non-vein and venule tissues, pathogen-induced degradation of cellulose and pectin and tree-initiated lignification of cell walls in response, amongst others, in lateral vein and mid-vein tissues. Via our developed computational algorithm, the underlying biomolecular differences between classes were identified and allowed accurate and rapid classification of disease with high accuracy of 69.6% for non-vein, 73.5% for venule, 82.1% for lateral vein and 85.6% for mid-vein tissues. Interfacial wetting differences between non-mildew covered and mildew-covered tissue were further analysed on the surfaces of non-vein and venule tissue. The overall results demonstrated the ability of Raman spectroscopy, combined with advanced AI, to act as a powerful and specific tool to probe foliar interactions between forest pathogens and host trees with the simultaneous potential to probe and catalogue molecular interactions between biological soft matter, paving the way for exploring similar relations in broader forest tree-pathogen systems.

In vitro studies of actin filament networks crosslinked with dynamic actin binding proteins provide critical insights into cytoskeletal mechanics as well as inspiration for new adaptive materials design. However, discontinuous variance in the physiochemical properties of actin binding proteins impedes holistic relationships between crosslinker molecular parameters, network structure, and mechanics. Bio-synthetic constructs composed of synthetic polymer backbones and actin binding motifs would enable crosslinkers with engineered physiochemical properties to directly target the desired structure–property relationships. As a proof of concept, bio-synthetic crosslinkers composed of highly flexible polyethylene glycol (PEG) polymers functionalized with the actin binding peptide LifeAct, are explored as actin crosslinkers. Using bulk rheology and fluorescence microscopy, these constructs are shown to modulate actin filament network structure and mechanics in a contour length dependent manner, while maintaining the stress-stiffening behavior inherent to actin filament networks. These results encourage the design of more diverse and complex peptide-polymer crosslinkers to interrogate and control semi-flexible polymer networks.

Enzyme-loaded spherical microgels with diameters of several micrometers have been explored for use in therapeutic microreactors and biosensors. Conventional preparation strategies for enzyme-loaded microgels utilized water-in-oil emulsions or flow chemistry techniques. The former damage enzyme activity using organic solvents and the latter are expensive and difficult to expand because of the complex system. In this study, we present a simple strategy for creating multiple enzyme-loaded gelatin-based microgels with tunable diameters in a single flask. This strategy was based on our finding that enzymes spontaneously partitioned in a dispersed methacryloyl gelatin aqueous solution in a poly(vinylpyrrolidone) (WGelMA/WPVP) aqueous solution. The method achieved an encapsulation efficiency of over 70% even with four types of enzymes and retained their activity owing to the full aqueous system. Additionally, the encapsulated β-galactosidase activity was maintained for 24 hours at pH 6, although naked β-galactosidase lost approximately 60% of its activity, which was superior to that of previous enzyme-loaded gelatin gels. Moreover, this simple method enabled the production of 10 g-scale or more microgels in one batch. We also demonstrated that multiple enzyme-loaded gelatin microgels functioned as cascade microreactors for lactose and glucose sensing. This versatile strategy enables the production of enzyme-loaded microgels while maintaining the enzyme activity using very low technologies. This result contributes to the easy preparation of enzyme-loaded microgels and their applications in the biomedical and green catalytic fields.

Liquid metal particulate composites (LMPCs) are super-stretchable conductors with promising applications in soft electronics. Their conductance originates from the percolation networks of liquid metal particles. This work aims at elucidating the effect of finite-size and sample shape on the percolation and electromechanical properties of LMPCs, given that their dimensions range from microns to centimeters. It is found that their percolation threshold is dominated by the smallest dimension of the samples, not the shape or aspect ratio. A smaller sample size increases the percolation threshold and makes it harder to activate the conductance. In addition, smaller samples are more sensitive to local defects, which adversely impair the electromechanical properties or even undermine the conductance. Finally, this work considers the influence of finite-size on the piezoresistance effect, i.e., strain-dependent resistance. It is found that the piezoresistance effect and finite-size effect are uncorrelated, if the samples are above the percolation threshold. The findings provide not only fundamental insights on the finite-size effect of percolation but also guidance on the design-fabrication process for LMPCs to achieve more reliable electromechanical performance.

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Using polyvinyl alcohol (PVA) and perylene-3,9-dicarboxylic acid (PDA) as raw materials, a new anti-freeze (−50 °C) fluorescent organogel with rapid shape-forming (2 h) properties was synthesised based on a certain proportion of the binary solvent of N,N-dimethylformamide (DMF) and dimethyl sulfoxide (DMSO). Then, an artificial light-harvesting system (ALHS) used in extremely cold environments was successfully constructed by mixing fluorescent dyes sulphorhodamine101 (SR101) and rhodamine 6G (R6G) into them as acceptors.

Exploiting the interplay of anisotropic diamagnetic susceptibility of liquid crystalline monomers and site selective photopolymerization enables the fabrication of 3D freeforms with highly refined microstructures. Utilizing chain transfer agents in the mesogenic inks presents a pathway for broadly tuning the mechanical properties of liquid crystalline polymers and their response to stimuli. In particular, the combination of 1,4-benzenedimethanethiol and tetrabromomethane is shown to enable voxelated blueprinting of molecular order, while allowing for a modulation of the crosslink density and the mechanical properties. The formulation of these monomers allows for the resolution of the voxels to approach the limits set by the coherence lengths defined by the anchoring from surfaces. These compositions demonstrate the expected thermotropic responses while allowing for their functionalization with photochromic switches to elicit photomechanical responses. Actuation strains are shown to outstrip that accomplished with prior systems that did not access chain transfer agents to modulate the structure of the macromolecular network. Test cases of this system are shown to create freeform actuators that exploit the refined director patterns during high-resolution printing. These include topological defects, hierarchically-structured light responsive grippers, and biomimetic flyers whose flight dynamics can be actively modulated via irradiation with light.

Predicting the behaviour of solutions with surfactants of significantly different critical micelle concentration (CMC) values remains a challenge. The study of the molecular interactions within micelles and interfaces in surfactant combinations used in everyday products is essential to understand these complex systems. In this work, the equilibrium and dynamic surface tension in the presence of mixed non-ionic (tristyrylphenol ethoxylates) and anionic (sodium benzene sulfonate with alkyl chain lengths of C10–C13) surfactants, commonly encountered as delivery systems in agrochemicals, were studied and their CMC values were determined. For the surfactant mixtures, four molar ratios were examined: nEOT/nNaDDBS = 0.01, 0.1, 1, 4 and two different cases were analysed, the premixed and the add one by one surfactant. The surface tension for single surfactants stabilised quickly, while the mixtures needed a long time to reach equilibrium; up to 15 h for the premixed mixtures and 40 min when surfactants were added one by one. The CMC values for the nEOT/nNaDDBS = 0.01, 0.1 premixed surfactant mixtures were found to be in between the CMC values of the single surfactants, but those for the nEOT/nNaDDBS = 1 and 4 mixtures were lower than the CMCs of both single surfactants. Calculations based on the regular solution theory suggested that there are attractive forces in the mixed micelles and at the interface layers, while the supramolecular assemblies in the bulk (i.e., micelles) and at interfaces (surfactant films) are preferentially enriched in EOT.

The formation and budding of lipid droplets (LDs) are known to be governed by the LD size and by membrane tensions in the endoplasmic reticulum (ER) bilayer and LD-monolayers. Using coarse-grained simulations of an LD model, we first show that ER-embedded LDs of different sizes can form through a continuous transition from wide LD lenses to spherical LDs at a fixed LD size. The ER tendency to relax its bilayer modulates the transition via a subtle interplay between the ER and LD lipid densities. By calculating the energetic landscape of the LD transition, we demonstrate that this size-independent transition is regulated by the mechanical force balance of ER and LD-tensions, independent from membrane bending and line tension whose energetic contributions are negligible according to our calculations. Our findings explain experimental observation of stable LDs of various shapes. We then propose a novel mechanism for directional LD budding where the required membrane asymmetry is provided by the exchange of lipids between the LD-monolayers. Remarkably, we demonstrate that this budding process is energetically neutral. Consequently, LD budding can proceed by a modest energy input from proteins or other driving agents. We obtain equal lipid densities and membrane tensions in LD-monolayers throughout budding. Our findings indicate that unlike LD formation, LD budding by inter-monolayer lipid exchange is a tension-independent process.

We numerically investigate the hydrodynamics and membrane dynamics of a multicomponent vesicle in two strongly confined geometries. This serves as a simplified model for red blood cells undergoing large deformations while traversing narrow constrictions. We propose a new parameterization for the bending modulus that remains positive for all lipid phase parameter values. For a multicomponent vesicle passing through a stenosis, we establish connections between various properties: lipid phase coarsening, size and flow profile of the lubrication layers, excess pressure, and the tank-treading velocity of the membrane. For a multicomponent vesicle passing through a contracting channel, we find that the lipid always phase separates so that the vesicle is stiffer in the front as it passes through the constriction. For both cases of confinement we find that lipid coarsening is arrested under strong confinement, and resumes at a high rate upon relief from extreme confinement. The results may be useful for efficient sorting lipid domains using microfluidic flows by controlled release of vesicles passing through strong confinement.

The adsorption of active polymers on an attractive nanoparticle (NP) is studied using Langevin dynamics simulations. The active polymers consist of an active Brownian particle (ABP) at the head and a subsequent passive polymer chain. The ABP experiences an active force of magnitude Fa. The interactions between the active polymer and NP are modeled as Lennard-Jones potential with a strength εpn. We find the critical adsorption point εpn* increases with increasing the active force Fa. The increment of εpn*, denoted as Δεpn*, due to Fa can be expressed approximately as Δεpn* ∝ Fa2.5 for the restricted rotating active polymer (RRAP) where the rotation of the head ABP is restricted and Δεpn* ∝ Fa1.7 for the freely rotating active polymer (FRAP) where the ABP rotates freely. Meanwhile, the conformation of the adsorbed polymer, such as adsorbed trains on NP and the tail near the ABP, are also dependent on Fa. When the tail near the ABP is short, the adsorption is significantly affected by the active force. However, when the tail is long, the whole polymer can be viewed as a long tail stretched by the active force and unperturbed adsorption monomers. Simulation results show that the active force has a direct and significant effect on εpn* and the structure of the adsorbed active polymers.

The aim of this study was to assess how transglutaminase (TG) impacts the microstructure, texture, and rheological properties of fermentation-induced pea protein emulsion gels. Additionally, the study examined the influence of storage time on the functional properties of these gels. Fermentation-induced pea protein gels were produced in the presence or absence of TG and stored for 1, 4, 8, 12, and 16 weeks. Texture analysis, rheological measurements, moisture content and microstructure evaluation with confocal laser scanning microscopy (CLSM) and 3D image analysis were conducted to explore the effects of TG on the structural and rheological properties of the fermented samples. The porosity of the protein networks in the pea gels decreased in the presence of TG, the storage modulus increased and the textural characteristics were significantly improved, resulting in harder and more springy gels. The gel porosity increased in gels with and without TG after storage but the effect of storage on textural and rheological properties was limited, indicating limited structural rearrangement once the fermentation-induced pea protein emulsion gels are formed. Greater coalescence was observed for oil droplets within the gel matrix after 16 weeks of storage in the absence of TG, consistent with these protein structures being weaker than the more structurally stable TG-treated gels. This study shows that TG treatment is a powerful tool to enhance the textural and rheological properties of fermentation-induced pea protein emulsion gels.

Multi-stimuli responsive photonic hydrogels (MRPHs) fabricated by doping nanoparticles into hydrogels show promising potential value in the fields of visual detection and drug delivery. However, complicated surface chemical modification is selected to improve the compatibility between nanoparticles and a pre-gel solution of hydrogel. Herein, we developed a simple and convenient vertical deposition method to prepare a novel photonic crystal (PC) template containing gold nanorods (Au NRs) (Au NRs/PC template), which could respond to near-infrared (NIR) light due to the conversion capability of Au NRs from NIR light to heat. Additionally, carboxyl groups on the surface of polystyrene (PS) colloids endowed the Au NRs/PC template with pH-stimulus responsiveness. Based on the Au NRs/PC template, MRPH film was fabricated by infiltrating the pre-gel solution of poly(N-isopropylacrylamide) (PNIPAM) hydrogel into the gap of a ‘sandwich’ structure through capillary forces and then polymerizing at 25 °C for 24 h. The obtained MRPH film could respond to NIR light, pH and temperature. Under the irradiation of NIR light, only the irradiated position lost structural color while the film volume had no distinct change. With the increase of ambient temperature, the whole MRPH film completely lost structural color and shrank significantly, which was greatly different from the phenomenon irradiated by NIR light. Besides, the structural color of the MRPH film exhibited a red shift from green to orange-red as the pH increased. Overall, both the Au NRs/PC template and the MRPH film may have potential applications in visual detection, due to their multi-stimuli responsiveness.

Recent experiments [S. H. Hashemi et al., Phys. Rev. Lett., 2018, 121, 185504] have shown that a long-ranged steady electric field emerges when applying an oscillating voltage over an electrolyte with unequal mobilities of cations and anions confined between two planar blocking electrodes. To explain this effect we analyse full numerical calculations based on the Poisson–Nernst–Planck equations by means of analytically constructed equivalent electric circuits. Surprisingly, the resulting equivalent circuit has two capacitive elements, rather than one, which introduces a new timescale for electrolyte dynamics. We find a good qualitative agreement between the numerical results and our simple analytic model, which shows that the long-range steady electric field emerges from the different charging rates of cations and anions in the electric double layers.

Correction for ‘Pure measures of bending for soft plates’ by Epifanio G. Virga, Soft Matter, 2024, http://doi.org/10.1039/D3SM01123B.

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Herein, the adsorption of polystyrene (PS) on phenyl-modified SiO2–Si substrates was investigated. Different from those for PS adsorption on a neat SiO2–Si substrate, the growth rate (vads) in the linear regime and hads/Rg (hads, thickness of flattened and loosely adsorbed layers on the substrate; Rg, radius of gyration) declined with increasing molecular weight (Mw) of PS and the phenyl content on the modified substrates, while the thickness of the flattened layer (hflat) and its coverage increased with increasing phenyl content. The results indicated that the adsorption of loose chains was controlled by the adsorption of flattened chains, as it only occurred in the empty contact sites remaining after the adsorption of flattened chains. Before approaching quasi-equilibrium (t < tcross), the number of flattened chain contact sites increased due to an enthalpically favorable process and, correspondingly, their spatial positions dynamically changed, which perturbed the adsorption of loose chains. When the adsorption of flattened chains reached quasi-equilibrium (t > tcross), the adsorption of loose chains was determined by the empty contact sites. The coverage of flattened chains and time to reach quasi-equilibrium were increased with more phenyl groups on the substrate, enhancing π–π interfacial interactions and resulting in a decreased adsorption rate and fewer loosely adsorbed chains. Mw-dependent vads and hads/Rg differed on phenyl-modified substrates compared to the neat SiO2–Si substrate owing to fewer empty contact sites for loose chains. The study findings improve our understanding of the mechanism responsible for the formation and structure of the adsorbed layer on solid surfaces.

Extensibility is beyond the paradigm of classical soft glassy materials, and more broadly, yield-stress fluids. Recently, model yield-stress fluids with significant extensibility have been designed by adding polymeric phases to classically viscoplastic dispersions [Nelson et al., J. Rheol., 2018, 62, 357; Nelson et al., Curr. Opin. Solid State Mater. Sci., 2019, 23, 100758; Dekker et al., J. Non-Newtonian Fluid Mech., 2022, 310, 104938]. However, fundamental questions remain about the design of and coupling between the shear and extensional rheology of such systems. In this work, we propose a model material, a mixture of soft glassy microgels and solutions of high molecular weight linear polymers. We establish systematic criteria for the design and thorough rheological characterization of such systems, in both shear and extension. Using our material, we show that it is possible to dramatically change the behavior in extension with minimal change in the shear yield stress and elastic modulus, thus enabling applications that exploit orthogonal modulation of shear and extensional material properties.

The pair-distribution function, which provides information about correlations in a system of interacting particles, is one of the key objects of theoretical soft matter physics. In particular, it allows for microscopic insights into the phase behavior of active particles. While this function is by now well studied for two-dimensional active matter systems, the more complex and more realistic case of three-dimensional systems is not well understood by now. In this work, we analyze the full pair-distribution function of spherical active Brownian particles interacting via a Weeks–Chandler–Andersen potential in three spatial dimensions using Brownian dynamics simulations. Besides extracting the structure of the pair-distribution function from the simulations, we obtain an analytical representation for this function, parametrized by activity and concentration, which takes into account the symmetries of a homogeneous stationary state. Our results are useful as input to quantitative models of active Brownian particles and advance our understanding of the microstructure in dense active fluids.