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Soft Matter

Carl C L Schuurmans, Anna Abbadessa, Mikkel A Bengtson, Galja Pletikapic, Huseyin Burak Eral, Gijsje Koenderink, Rosalinde Masereeuw, Wim E Hennink, Tina Vermonden
Glycosaminoglycans (GAGs) are of interest for biomedical applications because of their ability to retain proteins (e.g. growth factors) involved in cell-to-cell signaling processes. In this study, the potential of GAG-based microgels for protein delivery and their protein release kinetics upon encapsulation in hydrogel scaffolds were investigated. Monodisperse hyaluronic acid methacrylate (HAMA) and chondroitin sulfate methacrylate (CSMA) micro-hydrogel spheres (diameters 500-700 μm), were used to study the absorption of a cationic model protein (lysozyme), microgel (de)swelling, intra-gel lysozyme distribution and its diffusion coefficient in the microgels dispersed in buffers (pH 7...
July 19, 2018: Soft Matter
M Schulz, J L Keddie
For a wide range of applications, films are deposited from colloidal particles suspended in a volatile liquid. There is burgeoning interest in stratifying colloidal particles into separate layers within the final dry film to impart properties at the surface different to the interior. Here, we outline the mechanisms by which colloidal mixtures can stratify during the drying process. The problem is considered here as a three-way competition between evaporation of the continuous liquid, sedimentation of particles, and their Brownian diffusion...
July 19, 2018: Soft Matter
X Shao, J R Saylor, J B Bostwick
Mechanically-excited waves appear as surface patterns on soft agarose gels. We experimentally quantify the dispersion relationship for these waves over a range of shear modulus in the transition zone where the surface energy (capillarity) is comparable to the elastic energy of the solid. Rayleigh waves and capillary-gravity waves are recovered as limiting cases. Gravitational forces appear as a pre-stress through the self-weight of the gel and are important. We show the experimental data fits well to a proposed dispersion relationship which differs from that typically used in studies of capillary to elastic wave crossover...
July 19, 2018: Soft Matter
Vasilii Triandafilidi, Savvas G Hatzikiriakos, Jörg Rottler
We present a molecular dynamics study of two polyelectrolyte gels with different degrees of ionization coupled in a slab geometry. Our simulations show that a pressure gradient emerges between the two gels that results in the buildup of a Nernst-Donnan potential. This methodology is reverse to experiments of the piezoionic or mechanoelectric effect, in which an electric potential gradient appears upon application of a pressure gradient to a hydrogel. The Nernst-Donnan potential at the interface is found to scale linearly with temperature with the coefficient of proportionality given by the fraction of concentrations of the uncondensed counterions...
July 19, 2018: Soft Matter
Jian Li, Viacheslav Slesarenko, Stephan Rudykh
We investigate the instability-induced pattern transformations in 3D-printed soft composites consisting of stiff inclusions and voids periodically distributed in a soft matrix. These soft auxetic composites are prone to elastic instabilities giving rise to negative Poisson's ratio (NPR) behavior. Upon reaching the instability point, the composite microstructure rearranges into a new morphology attaining an NPR regime. Remarkably, identical composites can morph into distinct patterns depending on the loading direction...
July 19, 2018: Soft Matter
Lijuan Shi, Fenglin Liu, Tingting Liu, Jingsi Chen, Shaobo Xu, Hongbo Zeng
A smart gemini supra-amphiphile behaving with pH/CO2 dual-sensitive hierarchical self-assembly was fabricated under the effect of dynamic covalent bonds. In the presence of an amino-functionalized cation, water-insoluble terephthalaldehyde, and an amphiphilic anion, the benzoic imine bond can initiate the transformation from a single-tailed supra-amphiphile to a gemini supra-amphiphile with increasing pH, followed by the subsequent evolution from micelles to vesicles. Reversible self-assembly and disassembly of the gemini supra-amphiphile can be realized via CO2/N2 treatment, thus inducing the fission and reversion of vesicles...
July 18, 2018: Soft Matter
Edward D H Mansfield, Matthias Hartlieb, Sylvain Catrouillet, Julia Y Rho, Sophie C Larnaudie, Sarah E Rogers, Joaquin Sanchis, Johannes C Brendel, Sébastien Perrier
Self-assembling cyclic peptides (CP) consisting of amino acids with alternating d- and l-chirality form nanotubes by hydrogen bonding, hydrophobic interactions, and π-π stacking in solution. These highly dynamic materials are emerging as promising supramolecular systems for a wide range of biomedical applications. Herein, we discuss how varying the polymer conformation (linear vs. brush), as well as the number of polymer arms per peptide unimer affects the self-assembly of PEGylated cyclic peptides in different solvents, using small angle neutron scattering...
July 18, 2018: Soft Matter
Yang Yu, Fei Lu, Na Sun, Aoli Wu, Wei Pan, Liqiang Zheng
A promising method of synthesizing a lithium-containing room temperature polymeric ionic liquid (PIL) by utilizing the zwitterionic effect to turn a lithium salt into a liquid for single lithium-ion conduction was proposed. In this work, the room temperature PIL was constructed by the equimolar monomer mixture of zwitterion 3-(1-vinyl-3-imidazolic)propanesulfonate (VIPS) and 4-styrenesulfnny(trifluoromethylsulfony)imde (LiSTFSI) based on intermolecular electrostatic interactions. In situ photopolymerization with flexible chain poly(ethylene glycol)methyl ether methacrylate (PEGM) and cross-linker poly(ethylene glycol)dimethacrylate (PEGDM) in the presence of propylene carbonate (PC) generated free-standing PIL electrolyte films...
July 17, 2018: Soft Matter
Masoud Hoore, François Yaya, Thomas Podgorski, Christian Wagner, Gerhard Gompper, Dmitry A Fedosov
Red blood cell (RBC) aggregates play an important role in determining blood rheology. RBCs in plasma or polymer solution interact attractively to form various shapes of RBC doublets, where the attractive interactions can be varied by changing the solution conditions. A systematic numerical study on RBC doublet formation is performed, which takes into account the shear elasticity of the RBC membrane due to the spectrin cytoskeleton, in addition to the membrane bending rigidity. RBC membranes are modeled by two-dimensional triangular networks of linked vertices, which represent three-dimensional cell shapes...
July 17, 2018: Soft Matter
Evan Pretti, Hasan Zerze, Minseok Song, Yajun Ding, Nathan A Mahynski, Harold W Hatch, Vincent K Shen, Jeetain Mittal
Binary superlattices constructed from nano- or micron-sized colloidal particles have a wide variety of applications, including the design of advanced materials. Self-assembly of such crystals from their constituent colloids can be achieved in practice by, among other means, the functionalization of colloid surfaces with single-stranded DNA sequences. However, when driven by DNA, this assembly is traditionally premised on the pairwise interaction between a single DNA sequence and its complement, and often relies on particle size asymmetry to entropically control the crystalline arrangement of its constituents...
July 17, 2018: Soft Matter
Rachel Ramirez, Jerimiah Woodcock, S Michael Kilbey
Modifying the composition of polyampholytes, which are comprised of charge-positive and charge-negative repeat units, directly contributes to trade-offs between charge and structure, which are externally regulated by solution pH and added salt. Here, the relative ratio of anionic and cationic comonomers is varied to tailor the stimuli-responsiveness of poly(methacrylic acid-co-N,N-diethylaminoethyl methacrylate) (P(MAA-co-DEAEMA)) brushes to changes in solution pH and an added zwitterion. These systems display a strong dependence on excess repeating units of either type and the random incorporation appears to facilitate self-neutralization of charges...
July 17, 2018: Soft Matter
Matthew Mulvee, Natasa Vasiljevic, Stephen Mann, Avinash J Patil
Photo-generated nitric oxide radicals (NO˙) derived from sodium nitroprusside dihydrate (SNP) are employed for the construction of supramolecular hydrogels based on an amino acid derivative precursor, N-fluorenylmethyloxycarbonyl tyrosine phosphate (FYP), which through dephosphorylation produces the gelator, N-fluorenylmethyloxycarbonyl tyrosine (FY). Self-assembly of the amphiphilic gelator yields high-aspect ratio nanofilaments that entangle to form self-supporting, viscoelastic hydrogels. The presence of photolyzed SNP yields periodically twisted nanofilaments with opposite chirality to filaments formed through conventional hydrogelation routes...
July 16, 2018: Soft Matter
Charley Schaefer, René A J de Bruijn, Tom C B McLeish
The binding of ligands to distinct sites at proteins or at protein clusters is often cooperative or anti-cooperative due to allosteric signalling between those sites. The allostery is usually attributed to a configurational change of the proteins from a relaxed to a configurationally different tense state. Alternatively, as originally proposed by Cooper and Dryden, a tense state may be achieved by merely restricting the thermal vibrations of the protein around its mean configuration. In this work, we provide theoretical tools to investigate fluctuation allostery using cooling and titration experiments in which ligands regulate dimerisation, or ring or chain formation...
July 16, 2018: Soft Matter
Anand Narayanan Krishnamoorthy, Christian Holm, Jens Smiatek
We present the results of atomistic molecular dynamics simulations with regard to specific ion effects in water, methanol and N,N-dimethylacetamide (DMAc). As a reference system, we introduce rigid and rod-like models of polyanions and polycations in combination with alkali metal cations and halide anions as counterions. Pronounced specific ion effects can be observed in terms of the individual anion and cation condensation behavior. The outcomes of our simulations thus reveal significant deviations from standard electrostatic mean-field theories...
July 16, 2018: Soft Matter
A Brzyska, W Płaziński, K Woliński
In this work we use the Enforced Geometry Optimization (EGO) approach to simulate force-induced structural changes in the monomer, and di- up to pentameric oligomers of neutral and non-sulfated carrageenan based oligosaccharides. Our results indicate that the monosaccharide unit sequence in the oligomeric structure determines: (i) the type(s) of the enforced conformational transition(s), and (ii) the mechanical resistance to external forces. It is a direct consequence of the different glycosidic bonding types in the examined carregeenan based oligosaccharides...
July 13, 2018: Soft Matter
George R Heath, Patrick L Harrison, Peter N Strong, Stephen D Evans, Keith Miller
Understanding the mechanism of action of antimicrobial peptides (AMP) is fundamental to the development and design of peptide based antimicrobials. Utilizing fast-scan atomic force microscopy (AFM) we detail the attack of an AMP on both prototypical prokaryotic (DOPC:DOPG) and eukaryotic (DOPC:DOPE) model lipid membranes on the nanoscale and in real time. Previously shown to have a favourable therapeutic index, we study Smp43, an AMP with a helical-hinge-helical topology isolated from the venom of the North African scorpion Scorpio maurus palmatus...
July 12, 2018: Soft Matter
Pritha Dolai, Aditi Simha, Shradha Mishra
We study binary mixtures of small active and big passive athermal particles interacting via soft repulsive forces on a frictional substrate. Athermal self propelled particles are known to phase separate into a dense aggregate and a dilute gas-like phase at fairly low packing fractions. Known as motility induced phase separation, this phenomenon governs the behaviour of binary mixtures for small to intermediate size ratios of the particle species. An effective attraction between passive particles, due to the surrounding active medium, leads to true phase separation for large size ratios and volume fractions of active particles...
July 12, 2018: Soft Matter
Yulong Chen, Qian Xu, Yangfu Jin, Xin Qian, Rui Ma, Jun Liu, Dexin Yang
Coarse-grained Langevin dynamics simulations were performed to investigate the alignment behavior of monolayer films of cylinder-forming diblock copolymers under steady shear, a structure of significant importance for many technical applications such as nanopatterning. The influences of shear conditions, the interactions involved in the films, and the initial morphology of the cylinder-forming phase were examined. Our results showed that above a critical shear rate, the cylinders can align either along the shearing direction or transverse (log-rolling) to the shearing direction depending on the relative strength between the interchain attraction in the cylinders (εAA) and the surface attraction of the confining walls with the film (εBW)...
July 12, 2018: Soft Matter
Praveen Kumar, Prabhat Prakash, K R Ramya, Arun Venkatnathan
In this investigation, we examine the effect of water concentration and temperature on the dynamical properties of [Hmim][Cl] and [Hmim][NTf2] ionic liquids (ILs). The dynamical properties such as translational diffusion coefficients, ion-pair lifetimes, and rotational correlation times are calculated using molecular dynamics simulations. The simulations predict that water concentration also significantly impacts the magnitude of dynamical properties. At low, intermediate and high water concentrations, the following trend in diffusion coefficients is seen: Cl- > Hmim+; Cl- > NTf2-; Hmim+ ([Hmim][Cl]) > Hmim+ ([Hmim] [NTf2])...
July 12, 2018: Soft Matter
Steven Gottlieb, Dimitrios Kazazis, Iacopo Mochi, Laura Evangelio, Marta Fernández-Regúlez, Yasin Ekinci, Francesc Perez-Murano
Extreme ultraviolet interference lithography (EUV-IL) is used to manufacture topographical guiding patterns to direct the self-assembly of block copolymers. High-accuracy silicon oxide-like patterns with trenches ranging from 68 nm to 117 nm width are fabricated by exposing a hydrogen silsesquioxane (HSQ) resist layer using EUV-IL. We investigate how the accuracy, the low line width roughness and the low line edge roughness of the resulting patterns allow achieving DSA line/space patterns of a PS-b-PMMA (polystyrene-block-poly methyl methacrylate) block copolymer of 11 nm half-pitch with low defectivity...
July 12, 2018: Soft Matter
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