RESUMEN

The analysis of the impact of the star polymer topology on depletion interaction potentials, depletion forces, and monomer density profiles is carried out analytically using field theory methods and techniques as well as molecular dynamic simulations. The dimensionless depletion interaction potentials and the dimensionless depletion forces for a dilute solution of ideal star polymers with three and five legs (arms) in a Θ-solvent confined in a slit between two parallel walls with repulsive surfaces and for the case where one of the surfaces is repulsive and the other inert are obtained. Furthermore, the dimensionless layer monomer density profiles for ideal star polymers with an odd number (f˜ = 3, 5) of arms immersed in a dilute solution of big colloidal particles with different adsorbing or repelling properties in respect of polymers are calculated, bearing in mind the Derjaguin approximation. Molecular dynamic simulations of a dilute solution of star-shaped polymers in a good solvent with N = 901 (3 × 300 + 1 -star polymer with three arms) and 1501 (5 × 300 + 1 -star polymer with five arms) beads accordingly confined in a slit with different boundary conditions are performed, and the results of the monomer density profiles for the above-mentioned cases are obtained. The numerical calculation of the radius of gyration for star polymers with f˜ = 3, 5 arms and the ratio of the perpendicular to parallel components of the radius of gyration with respect to the wall orientation for the above-mentioned cases is performed. The obtained analytical and numerical results for star polymers with an odd number (f˜ = 3, 5) of arms are compared with our previous results for linear polymers in confined geometries. The acquired results show that a dilute solution of star polymer chains can be applied in the production of new functional materials, because the behavior of these solutions is strictly correlated with the topology of polymers and also with the nature and geometry of confined surfaces. The above-mentioned properties can find extensive practical application in materials engineering, as well as in biotechnology and medicine for drug and gene transmission.

Asunto(s)

RESUMEN

Block copolymers are recognized as a valuable platform for creating nanostructured materials. Morphologies formed by block copolymer self-assembly can be transferred into a wide range of inorganic materials, enabling applications including energy storage and metamaterials. However, imaging of the underlying, often complex, nanostructures in large volumes has remained a challenge, limiting progress in materials development. Taking advantage of recent advances in X-ray nanotomography, we noninvasively imaged exceptionally large volumes of nanostructured hybrid materials at high resolution, revealing a single-diamond morphology in a triblock terpolymer-gold composite network. This morphology, which is ubiquitous in nature, has so far remained elusive in block copolymer-derived materials, despite its potential to create materials with large photonic bandgaps. The discovery was made possible by the precise analysis of distortions in a large volume of the self-assembled diamond network, which are difficult to unambiguously assess using traditional characterization tools. We anticipate that high-resolution X-ray nanotomography, which allows imaging of much larger sample volumes than electron-based tomography, will become a powerful tool for the quantitative analysis of complex nanostructures and that structures such as the triblock terpolymer-directed single diamond will enable the generation of advanced multicomponent composites with hitherto unknown property profiles.

RESUMEN

Current mesh-based simulation approaches face significant challenges in continuously modeling the mechanical behaviors of foods through processing, storage, deconstruction, and digestion. This is primarily due to the limitations of continuum mechanics in dealing with systems characterized by free boundaries, substantial deformations, mechanical failures, and non-homogenized mechanical properties. The dynamic nature of food microstructure and the transformation of the food bolus, in relation to its composition, present formidable obstacles in computer-aided food design. In response, the Pizza3 project adopts an innovative methodology, utilizing an explicit microstructural representation to construct and subsequently deconstruct food products in a modular, Lego-like fashion. Central to this simulation approach are "food atoms", conceptualized from the principles of smoothed particle hydrodynamics. These units are significantly larger than actual atoms but are finely scaled to represent both solid and liquid states of food faithfully. In solid phases, food atoms interact via pairwise forces akin to bond-peridynamic methods, thus extending the capabilities of continuum mechanics to encompass large deformations and fracturing phenomena. For liquids, the model employs artificial conservative and dissipative forces, enabling the simulation of a variety of phenomena within the framework of partial compressibility. The interaction dynamics between rigid and soft objects and fluids are accurately captured through Hertzian contact mechanics, offering a versatile parameterization applicable to impermeable (but possibly penetrable) surfaces and enforcing no-slip conditions. The efficacy of this framework is showcased through the successful modeling of three time-dependent 3D scenarios, each rigorously validated against established analytical and experimental models. Advancing beyond these initial applications, the framework is further extended to more intricate cases inadequately addressed in current literature. This extension sheds light on the underlying mechanisms of in-mouth texture perception, offering new insights and tools for food engineering and design.

Asunto(s)

RESUMEN

Miniature robots are untethered actuators, which have great prospects to transform targeted drug delivery because they can potentially deliver high concentrations of medicine to the disease site(s) with minimal complications. However, existing miniature robots cannot perform advanced targeted combination therapy; majority of them can at most transport one type of drug, while those that can carry multiple drugs are unable to change their drug-dispensing sequence and dosage. Furthermore, the latter robots cannot transport more than three types of drugs, selectively dispense their drugs, maintain their mobility, or release their drugs at multiple sites. Here, a millimeter-scale soft robot is proposed, which can be actuated by alternating magnetic fields to dispense four types of drugs with reprogrammable drug-dispensing sequence and dosage (dispensing rates: 0.0992-0.231 µL h-1). This robot has six degrees-of-freedom motions, and it can deliver its drugs to multiple desired sites by rolling and two-anchor crawling across unstructured environments with negligible drug leakage. Such dexterity is highly desirable and unprecedented for miniature robots with drug-dispensing capabilities. The soft robot therefore has great potential to enable advanced targeted combination therapy, where four types of drugs must be delivered to various disease sites, each with a specific sequence and dosage of drugs.

RESUMEN

Memristors show promising features for neuromorphic computing. Here we report a soft memristor based on the liquid-vapor surface of a microbubble. The thickness of the liquid film was modulated by electrostatic and interfacial forces, enabling resistance switches. We found a pinched current hysteresis at scanning periods between 1.6 and 51.2 s, while representing a resistor below 1.6 s and a diode-like behavior above 51.2 s. We approximate the thickening/thinning dynamics of liquid film by pressure-driven flow at the interface and derived the impacts of salt concentration and voltage amplitude on the memory effects. Our work opens a new approach to building nanofluidic memristors by a soft interface, which may be useful for new types of neuromorphic computing in the future.

RESUMEN

HYPOTHESIS: In order to understand the basic mechanisms affecting emulsion stability, the intrinsic dynamics of the drop population must be investigated. We hypothesize that transient ballistic motion can serve as a marker of interactions between drops. In 1G conditions, buoyancy-induced drop motion obscures these interactions. The microgravity condition onboard the International Space Station enable this investigation. EXPERIMENTS: We performed Diffusing Wave Spectroscopy (DWS) experiments in the ESA Soft Matter Dynamics (SMD) facility. We used Monte Carlo simulations of photon trajectory to support data analysis. The analysis framework was validated by ground-based characterizations of the initial drop size distribution (DSD) and the properties of the oil/water interface in the presence of surfactant. FINDINGS: We characterized the drop size distribution and found to be bi-disperse. Drop dynamics shows transient ballistic features at early times, reaching a stationary regime of primarily diffusion-dominated motion. This suggests different ageing mechanisms: immediately after emulsification, the main mechanism is coalescence or aggregation between small drops. However at later times, ageing proceeds via coalescence or aggregation of small with large drops in some emulsions. Our results elucidate new processes relevant to emulsion stability with potential impact on industrial processes on Earth, as well as enabling technologies for space exploration.

RESUMEN

HYPOTHESIS: Soft materials, particularly elastomers, are extensively studied, but investigations into purely soft gel contact systems are limited due to their complex dual phases consisting of polymer and free liquids. While Dual Wavelength-Reflection Interference Confocal Microscopy (DW-RICM) is effective for noninvasively visualizing interfaces from a bottom view, it faces challenges in gel studies due to close refractive indices of polymeric networks and free liquids. We hypothesize that modulating the refractive index of soft gels using nanoparticles (NPs) enhances the visualization of contact zone beneath the free surface, providing insights into the configuration of phase-separated free oil within gel-on-gel contact systems. EXPERIMENTS: Gel-on-gel contact systems were fabricated using immiscible organogels and hydrogels. Titanium dioxide (TiO2) NPs were introduced into the organogel to modulate refractive indices. Given the lack of prior studies on the hidden contact zone between gels, various techniques, including DW-RICM, side-view imaging, and inverted optical microscopy, were employed to observe and validate our findings. Comparative analyses were conducted with elastomer-on-rigid, elastomer-on-gel, and gel-on-rigid contact systems. FINDINGS: Our investigation demonstrated that a minimal amount of TiO2 NPs effectively delineates the direct contact radius between organogel polymeric networks and hydrogel surfaces. Comparative experiments showed that TiO2 addition did not alter the gels' mechanical and surface properties but significantly enhanced information on gel contact deformation. This enhanced visualization technique has the potential to advance our understanding of adhesive contacts in gels, providing valuable insights into interface phenomena involving biological soft tissues and cells.

RESUMEN

Magnetically responsive soft smart materials have garnered significant academic attention due to their flexibility, remote controllability, and reconfigurability. However, traditional soft materials used in the construction of these magnetically responsive systems typically exhibit low density and poor thermal and electrical conductivities. These limitations result in suboptimal performance in applications such as medical radiography, high-performance electronic devices, and thermal management. To address these challenges, magnetically responsive gallium-based liquid metals have emerged as promising alternatives. In this review, we summarize the methodologies for achieving magnetically responsive liquid metals, including the integration of magnetic agents into the liquid metal matrix and the utilization of induced Lorentz forces. We then provide a comprehensive discussion of the key physicochemical properties of these materials and the factors influencing them. Additionally, we explore the advanced and potential applications of magnetically responsive liquid metals. Finally, we discuss the current challenges in this field and present an outlook on future developments and research directions.

RESUMEN

During embryonic morphogenesis, tissues undergo dramatic deformations in order to form functional organs. Similarly, in adult animals, living cells and tissues are continually subjected to forces and deformations. Therefore, the success of embryonic development and the proper maintenance of physiological functions rely on the ability of cells to withstand mechanical stresses as well as their ability to flow in a collective manner. During these events, mechanical perturbations can originate from active processes at the single-cell level, competing with external stresses exerted by surrounding tissues and organs. However, the study of tissue mechanics has been somewhat limited to either the response to external forces or to intrinsic ones. In this work, we use an active vertex model of a 2D confluent tissue to study the interplay of external deformations that are applied globally to a tissue with internal active stresses that arise locally at the cellular level due to cell motility. We elucidate, in particular, the way in which this interplay between globally external and locally internal active driving determines the emergent mechanical properties of the tissue as a whole. For a tissue in the vicinity of a solid-fluid jamming or unjamming transition, we uncover a host of fascinating rheological phenomena, including yielding, shear thinning, continuous shear thickening, and discontinuous shear thickening. These model predictions provide a framework for understanding the recently observed nonlinear rheological behaviors in vivo.

RESUMEN

Structural and functional explorations on bio-soft matter such as micelles, vesicles, nanoparticles, aggregates or polymers derived from traditional Chinese medicine (TCM) has emerged as a new topic in the field of TCM. The discovery of such cross-scaled bio-soft matter may provide a unique perspective for unraveling the new effective material basis of TCM as well as developing innovative medicine and biomaterials. Despite the rapid rise of TCM-derived bio-soft matter, their hierarchical structure and assembly mechanism must be unambiguously probed for a further in-depth understanding of their pharmacological activity. In this review, the current emerged TCM-derived bio-soft matter assembled from either small molecules or macromolecules is introduced, and particularly the unambiguous elucidation of their hierarchical structure and assembly mechanism with combined electron microscopic and spectroscopic techniques is depicted. The pros and cons of each technique are also discussed. The future challenges and perspective of TCM-derived bio-soft matter are outlined, particularly the requirement for their precise in situ structural determination is highlighted.

RESUMEN

Standard deep learning algorithms require differentiating large nonlinear networks, a process that is slow and power-hungry. Electronic contrastive local learning networks (CLLNs) offer potentially fast, efficient, and fault-tolerant hardware for analog machine learning, but existing implementations are linear, severely limiting their capabilities. These systems differ significantly from artificial neural networks as well as the brain, so the feasibility and utility of incorporating nonlinear elements have not been explored. Here, we introduce a nonlinear CLLN-an analog electronic network made of self-adjusting nonlinear resistive elements based on transistors. We demonstrate that the system learns tasks unachievable in linear systems, including XOR (exclusive or) and nonlinear regression, without a computer. We find our decentralized system reduces modes of training error in order (mean, slope, curvature), similar to spectral bias in artificial neural networks. The circuitry is robust to damage, retrainable in seconds, and performs learned tasks in microseconds while dissipating only picojoules of energy across each transistor. This suggests enormous potential for fast, low-power computing in edge systems like sensors, robotic controllers, and medical devices, as well as manufacturability at scale for performing and studying emergent learning.

RESUMEN

Complex materials that change their optical properties in response to changes in environmental conditions can find applications in displays, smart windows, and optical sensors. Here a class of biphasic composites with stimuli-adaptive optical transmittance is introduced. The biphasic composites comprise aqueous droplets (a mixture of water, glycerol, and surfactant) embedded in an elastomeric matrix. The biphasic composites are tuned to be optically transparent through a careful match of the refractive indices between the aqueous droplets and the elastomeric matrix. We demonstrate that stimuli (e.g., salinity and temperature change) can trigger variations in the optical transmittance of the biphasic composite. The introduction of such transparency-changing soft matter with liquid inclusions offers a novel approach to designing advanced optical devices, optical sensors, and metamaterials.

RESUMEN

A self-healing gel with self-healing kinetics that can be regulated by heat is developed. The gel is composed of a polymer having benzophenone (BP) substituents, which are cross-linked with a main alkyl chain via ester bonds, titanium chloride, and zinc. This gel material shows a self-healing property at room temperature. Also, its self-healing behavior can be accelerated by heating the gel. This gel having self-healing kinetics that can be regulated by heat is favorable for practical use. When we want to use a self-healing property as a stop-gap measure, a rapid self-healing property is demanded. On the other hand, when we want materials repaired beautifully or decomposed surfaces need to be attached beautifully, a slow self-healing property is favorable. These opposite demands can be answered by the gel with self-healing kinetics that can be regulated by heat.

RESUMEN

Embedded printing has emerged as a valuable tool for fabricating complex structures and microfluidic devices. Currently, an ample of amount of research is going on to develop new materials to advance its capabilities and increase its potential applications. Here, we demonstrate a novel, transparent, printable, photocrosslinkable, and tuneable silicone composite that can be utilized as a support bath or an extrudable ink for embedded printing. Its properties can be tuned to achieve ideal rheological properties, such as optimal self-recovery and yield stress, for use in 3D printing. When used as a support bath, it facilitated the generation microfluidic devices with circular channels of diameter up to 30 µm. To demonstrate its utility, flow focusing microfluidic devices were fabricated for generation of Janus microrods, which can be easily modified for multitude of applications. When used as an extrudable ink, 3D printing of complex-shaped constructs were achieved with integrated electronics, which greatly extends its potential applications towards soft robotics. Further, its biocompatibility was tested with multiple cell types to validate its applicability for tissue engineering. Altogether, this material offers a myriad of potential applications (i.e., soft robotics, microfluidics, bioprinting) by providing a facile approach to develop complicated 3D structures and interconnected channels.

RESUMEN

Axonal outgrowth, cell crawling, and cytokinesis utilize actomyosin, microtubule-based motors, cytoskeletal dynamics, and substrate adhesions to produce traction forces and bulk cellular motion. While it has long been appreciated that growth cones resemble crawling cells and that the mechanisms that drive cytokinesis help power cell crawling, they are typically viewed as unique processes. To better understand the relationship between these modes of motility, here, we developed a unified active fluid model of cytokinesis, amoeboid migration, mesenchymal migration, neuronal migration, and axonal outgrowth in terms of cytoskeletal flow, adhesions, viscosity, and force generation. Using numerical modeling, we fit subcellular velocity profiles of the motions of cytoskeletal structures and docked organelles from previously published studies to infer underlying patterns of force generation and adhesion. Our results indicate that, during cytokinesis, there is a primary converge zone at the cleavage furrow that drives flow towards it; adhesions are symmetric across the cell, and as a result, cells are stationary. In mesenchymal, amoeboid, and neuronal migration, the site of the converge zone shifts, and differences in adhesion between the front and back of the cell drive crawling. During neuronal migration and axonal outgrowth, the primary convergence zone lies within the growth cone, which drives actin retrograde flow in the P-domain and bulk anterograde flow of the axonal shaft. They differ in that during neuronal migration, the cell body is weakly attached to the substrate and thus moves forward at the same velocity as the axon. In contrast, during axonal outgrowth, the cell body strongly adheres to the substrate and remains stationary, resulting in a decrease in flow velocity away from the growth cone. The simplicity with which cytokinesis, cell crawling, and axonal outgrowth can be modeled by varying coefficients in a simple model suggests a deep connection between them.

RESUMEN

Although descended from orb weavers, spiders in the family Theridiidae spin cobwebs whose sticky prey capture gumfoot lines extend from a silk tangle to a surface below. When a crawling insect contacts glue droplets at the bottom of a gumfoot line, the line's weak pyriform anchor releases, causing the taut line to contract, pulling the insect from the surface and making its struggles to escape ineffective. To determine if this change in prey capture biomechanics was accompanied by a change in the material properties of theridiid glue, we characterized the elastic modulus and toughness of the glue droplet proteins of four theridiid species at 20-90 % relative humidity and compared their properties with those of 13 orb weaving species in the families Tetragnathidae and Araneidae. Compared to orb weavers, theridiid glue proteins had low extensions per protein volume and low elastic modulus and toughness values. These differences are likely explained by the loss of tension on a gumfoot line when its anchor fails, which may prioritize glue droplet adhesion rather than extension. Similarities in theridiid glue droplet properties did not reflect these species' evolutionary relationships. Instead, they appear associated with differences in web architecture. Two species that had stiffer gumfoot support lines and longer and more closely spaced gumfoot lines also had stiffer glue proteins. These lines may store more energy, and, when their anchors release, require stiffer glue to resist the more forceful upward thrust of a prey. STATEMENT OF SIGNIFICANCE: When a crawling insect contacts glue droplets on a theridiid cobweb's gumfoot line, this taut line's anchor fails and the insect is hoisted upward, rendering its struggles to escape ineffective. This strategy contrasts with that of orb weaving ancestors, which rely on more closely spaced prey capture threads to intercept and retain flying insects. A comparison of the elastic modulus and toughness of gumfoot and orb web glue proteins shows that this change in prey capture biomechanics is associated with reductions in the stiffness and toughness of cobweb glue. Unlike orb web capture threads, whose droplets extend in a coordinated fashion to sum adhesive forces, gumfoot lines become untethered, which prioritizes glue droplet adhesive contact over glue droplet extension.

Asunto(s)

RESUMEN

Polymer coating to substrates alters surface chemistry and imparts bulk material functionalities with a minute thickness, even in nanoscale. Specific surface modification of a substate usually requires an active substrate that, e.g., undergoes a chemical reaction with the modifying species. Here, we present a generic method for surface modification, namely, solid-state adsorption, occurring purely by entropic strive. Formed by heating above the melting point or glass transition and subsequent rinsing of the excess polymer, the emerging ultrathin (<10 nm) layers are known in fundamental polymer physics but have never been utilized as building blocks for materials and they have never been explored on soft matter substrates. We show with model surfaces as well as bulk substrates, how solid-state adsorption of common polymers, such as polystyrene and poly(lactic acid), can be applied on soft, cellulose-based substrates. Our study showcases the versatility of solid-state adsorption across various polymer/substrate systems. Specifically, we achieve proof-of-concept hydrophobization on flexible cellulosic substrates, maintaining irreversible and miniscule adsorption yet with nearly 100% coverage without compromising the bulk material properties. The method can be considered generic for all polymers whose Tg and Tm are below those of the to-be-coated adsorbed layer, and whose integrity can withstand the solvent leaching conditions. Its full potential has broad implications for diverse materials systems where surface coatings play an important role, such as packaging, foldable electronics, or membrane technology.

RESUMEN

Diffuse soft matter interfaces take many forms, from end-tethered polymer brushes or adsorbed surfactants to self-assembled layers of lipids. These interfaces play crucial roles across a multitude of fields, including materials science, biophysics, and nanotechnology. Understanding the nanostructure and properties of these interfaces is fundamental for optimising their performance and designing novel functional materials. In recent years, reflectometry techniques, in particular neutron reflectometry, have emerged as powerful tools for elucidating the intricate nanostructure of soft matter interfaces with remarkable precision and depth. This review provides an overview of selected recent developments in reflectometry and their applications for illuminating the nanostructure of diffuse interfaces. We explore various principles and methods of neutron and X-ray reflectometry, as well as ellipsometry, and discuss advances in their experimental setups and data analysis approaches. Improvements to experimental neutron reflectometry methods have enabled greater time resolution in kinetic measurements and elucidation of diffuse structure under shear or confinement, while innovation in analysis protocols has significantly reduced data processing times, facilitated co-refinement of reflectometry data from multiple instruments and provided greater-than-ever confidence in proposed structural models. Furthermore, we highlight some significant research findings enabled by these techniques, revealing the organisation, dynamics, and interfacial phenomena at the nanoscale. We also discuss future directions and potential advancements in reflectometry techniques. By shedding light on the nanostructure of diffuse interfaces, reflectometry techniques enable the rational design and tailoring of interfaces with enhanced properties and functionalities.

RESUMEN

We report the use of wet-spinning to 3D-print gels from low-molecular-weight gelators (LMWGs) based on the 1,3 : 2,4-dibenzylidenesorbitol (DBS) scaffold. Gel stripes assembled from DBS-CONHNH2 and DBS-COOH are printed, and their conductivities assessed. Printed gels based on DBS-CONHNH2 can be loaded with Au(III), which is reduced in situ to form embedded gold nanoparticles (AuNPs). The conductivity of these gels increases because of electron transport mediated by the AuNPs, whereas the conductivity of DBS-COOH, which does not promote AuNP formation, remains lower. We then fabricate multi-component gel patterns comprised of spatially well-defined domains of printed DBS-CONHNH2/AuNP (higher conductivity) and DBS-COOH (lower conductivity) resulting in soft multi-domain materials with differential conductivity. Such materials have future prospects in applications such as soft nanoelectronics or tissue engineering.

RESUMEN

Using a three-dimensional model of cell monolayers, we study the spatial organization of active stress chains as the monolayer transitions from a solid to a liquid state. The critical exponents that characterize this transition map the isotropic stress percolation onto the two-dimensional random percolation universality class, suggesting short-range stress correlations near this transition. This mapping is achieved via two distinct, independent pathways: (i) cell-cell adhesion and (ii) active traction forces. We unify our findings by linking the nature of this transition to high-stress fluctuations, distinctly linked to each pathway. The results elevate the importance of the transmission of mechanical information in dense active matter and provide a new context for understanding the non-equilibrium statistical physics of phase transition in active systems.

Asunto(s)