Bulletin of the American Physical Society
APS March Meeting 2016
Volume 61, Number 2
Monday–Friday, March 14–18, 2016; Baltimore, Maryland
Session R38: Biopolymers and Biohybrid Polymers: Networks and HydrogelsFocus
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Sponsoring Units: DPOLY DBIO GSOFT Chair: Bradley Olsen, MIT Room: 341 |
Thursday, March 17, 2016 8:00AM - 8:12AM |
R38.00001: Self-Healing Nanocomposite Hydrogel with Well-Controlled Dynamic Mechanics Qiaochu Li, Sumeet Mishra, Pangkuan Chen, Joseph Tracy, Niels Holten-Andersen Network dynamics is a crucial factor that determines the macroscopic self-healing rate and efficiency in polymeric hydrogel materials, yet its controllability is seldom studied in most reported self-healing hydrogel systems. Inspired by mussel's adhesion chemistry, we developed a novel approach to assemble inorganic nanoparticles and catechol-decorated PEG polymer into a hydrogel network. When utilized as reversible polymer-particle crosslinks, catechol-metal coordination bonds yield a unique gel network with dynamic mechanics controlled directly by interfacial crosslink structure. Taking advantage of this structure-property relationship at polymer-particle interfaces, we next designed a hierarchically structured hybrid gel with two distinct relaxation timescales. By tuning the relative contribution of the two hierarchical relaxation modes, we are able to finely control the gel's dynamic mechanical behavior from a viscoelastic fluid to a stiff solid, yet preserving its fast self-healing property without the need for external stimuli. [Preview Abstract] |
Thursday, March 17, 2016 8:12AM - 8:24AM |
R38.00002: Polymer-induced compression of biological hydrogels Sujit Datta, Asher Preska Steinberg, Rustem Ismagilov Hydrogels -- such as mucus, blood clots, and the extracellular matrix -- provide critical functions in biological systems. However, little is known about how their structure is influenced by many of the polymeric materials they come into contact with regularly. Here, we focus on one critically important biological hydrogel: colonic mucus. While several biological processes are thought to potentially regulate the mucus hydrogel structure, the polymeric composition of the gut environment has been ignored. We use Flory-Huggins solution theory to characterize polymer-mucus interactions. We find that gut polymers, including those small enough to penetrate the mucus hydrogel, can in fact alter mucus structure, changing its equilibrium degree of swelling and forcing it to compress. The extent of compression increases with increasing polymer concentration and size. We use experiments on mice to verify these predictions with common dietary and therapeutic gut polymers. Our results provide a foundation for investigating similar, previously overlooked, polymer-induced effects in other biological hydrogels. [Preview Abstract] |
Thursday, March 17, 2016 8:24AM - 8:36AM |
R38.00003: Thermal-induced ageing of agar solutions: impact on the structural and mechanical properties of agar gels Bosi Mao, Ahmed Bentaleb, Fr\'ed\'eric Louerat, Thibaut Divoux, Patrick Snabre Numerous hydrogels are prepared by cooling down to ambient temperature, aqueous polymer solutions brought to a boil. Although the incubation time of the polymer solution at such a high temperature could be used as a tuning parameter, its impact on the subsequent gelation has been poorly investigated. Here we study the effect of prolonged heating at 80$^{\circ}$C on a 1.5\% wt solution of agar, a natural polysaccharide. The incubation time is varied from a few hours up to five days. We show that the agar sol. continuously degrades as the result of both the hydrolysis and the intermolecular oxidation of the polymer chains. Furthermore, electronic microscopy and X-ray diffraction experiments reveal that gels formed from older agar sols display an increasingly coarser microstructure composed of micron-sized aggregated pieces of polysaccharides, in contrast with the fibrous-like structure of gels made from fresh sols. Along with structural changes prolonged incubation time leads to weaker gels of lower shear elastic modulus. Finally, macro-indentation experiments coupled to direct visualization show that increasing the incubation time of the agar sol. decreases the yield strain of the gel by a factor of three, while the rupture scenario turns continuously from brittle to ductile-like. [Preview Abstract] |
Thursday, March 17, 2016 8:36AM - 8:48AM |
R38.00004: Nonlinear elasticity of alginate gels Seyed Meysam Hashemnejad, Santanu Kundu Alginate is a naturally occurring anionic polysaccharide extracted from brown algae. Because of biocompatibility, low toxicity, and simple gelation process, alginate gels are used in biomedical and food applications. Here, we report the rheological behavior of ionically crosslinked alginate gels, which are obtained by in situ gelation of alginates with calcium salts, in between two parallel plates of a rheometer. Strain stiffening behavior was captured using large amplitude oscillatory shear (LAOS) experiments. In addition, negative normal stress was observed for these gels, which has not been reported earlier for any polysaccharide networks. The magnitude of negative normal stress increases with applied strain and can exceed that of the shear stress at large strain. Rheological results fitted with a constitutive model that considers both stretching and bending of chains indicate that nonlinearity is likely related to the stretching of the chains between the crosslink junctions. The results provide an improved understanding of the deformation mechanism of ionically crosslinked alginate gel and the results will be important in developing synthetic extracellular matrix (ECM) from these materials. [Preview Abstract] |
Thursday, March 17, 2016 8:48AM - 9:00AM |
R38.00005: Cryo-imaging and modeling of the super molecular structure of cross-linked gelatin and its applications. Clement MARMORAT, Arkadi Arinstein, Naama Koifman, Yeshayahu Talmon, Eyal Zussman, Miriam Rafailovich The need for naturally derived materials to synthetize bio-compatible scaffolds is growing. In its natural state, gelatin derives its properties from a network of structured, intertwined, triple helical chains. The mechanical properties can be further controlled by additional enzymatic cross-linking. But, in contrast to simple polymer systems, the response to an imposed deformation is then determined by two competing factors, the establishment of the cross-linked mesh vs. the self-assembly of the fibrils into larger and therefore stronger hierarchical structures. Properties deduced from the response functions to measurements; such as rheology or swelling, are then a combination of these two very different factors, hence impossible to model unless more precise knowledge is available regarding the internal structure. We applied cryogenic-temperature scanning electron microscopy (cryo-SEM) to image the networks. Based on these images, a theoretical model was developed, for which we obtained excellent agreement for the mesh size of both networks, and their mechanical properties. We then used these controlled scaffolds, embedding them with fluorescent beads, to image live cells traction forces at stake during cell migration. [Preview Abstract] |
Thursday, March 17, 2016 9:00AM - 9:12AM |
R38.00006: Encoding Mechano-Memories in Actin Networks louis foucard, Sayantan majumdar, Alex Levine, Margaret Gardel The ability of cells to sense and adapt to external mechanical stimuli is vital to many of its biological functions. A critical question is therefore to understand how mechanosensory mechanisms arise in living matter, with implications in both cell biology and smart materials design. Experimental work has demonstrated that the mechanical properties of semiflexible actin networks in Eukaryotic cells can be modulated (either transiently or irreversibly) via the application of external forces. Previous work has also shown with a combination of numerical simulations and analytic calculations shows that the broken rotational symmetry of the filament orientational distribution in semiflexible networks leads to dramatic changes in the mechanical response. Here we demonstrate with a combination of numerical and analytic calculations that the observed long-lived mechano-memory in the actin networks arise from changes in the nematic order of the constituent filaments. These stress-induced changes in network topology relax slowly under zero stress and can be observed through changes in the nonlinear mechanics. Our results provide a strategy for designing a novel class of materials and demonstrate a new putative mechanism of mechanical sensing in eukaryotic cells. [Preview Abstract] |
Thursday, March 17, 2016 9:12AM - 9:24AM |
R38.00007: Fibril Formation and Phase Separation in Aqueous Cellulose Ethers Amanda Maxwell, Peter Schmidt, John McAllister, Joseph Lott, Frank Bates, Timothy Lodge Aqueous solutions of many cellulose ethers are known to undergo thermoreversible gelation and phase separation upon heating to form turbid hydrogels, but the mechanism and resulting structures have not been well understood. Turbidity, light scattering and small-angle neutron scattering (SANS) are used to show that hydroxypropyl methylcellulose (HPMC) chains are dissolved in water below 50 $^{\circ}$C and undergo phase separation at higher temperatures. At 70 $^{\circ}$C, at sufficiently high concentrations in water, HPMC orders into fibrillar structures with a well-defined radius of 18 $\pm$ 2 nm, as characterized by cryogenic transmission electron microscopy and SANS. The HPMC fibril structure is independent of concentration and heating rate. However, HPMC fibrils do not form a percolating network as readily as is seen in methylcellulose, resulting in a lower hot-gel modulus, as demonstrated by rheology. [Preview Abstract] |
Thursday, March 17, 2016 9:24AM - 9:36AM |
R38.00008: Simulation of Polymer Physical Gel With Platelet Fillers Di Xu, Dilip Gerssape Platelet filler such as clays have superior effects on the properties of polymer gels. We used molecular dynamic simulations to study platelet filled composite gels system, in which small hexagonal disks simulate the platelets and gelation is due to short-range attraction between end-monomers and platelets. The properties of platelet filled composites are studied as a function of filler concentration. The mechanism of gelation was found similar to those of pure polymer gels; the polymers and platelets formed organic-inorganic networks, which percolate at high enough filler concentration. It was observed platelets aggregated into local intercalation structure, which significantly differs from typical spherical fillers. This unique intercalation structure is examined by radial distribution function and ordering parameters. We discussed how intercalation would affect the properties of the platelet composites by comparing them with spherical fillers. [Preview Abstract] |
Thursday, March 17, 2016 9:36AM - 9:48AM |
R38.00009: A Coarse-Grained Model for Simulating Chitosan Hydrogels Hongcheng Xu, Silvina Matysiak Hydrogels are biologically-derived materials composed of water-filled cross-linking polymer chains. It has widely been used as biodegradable material and has many applications in medical devices. The chitosan hydrogel is stimuli-responsive for undergoing pH-sensitive self-assembly process, allowing programmable tuning of the chitosan deposition through electric pulse. To explore the self-assembly mechanism of chitosan hydroge, we have developed an explicit-solvent coarse-grained chitosan model that has roots in the MARTINI force field, and the pH change is modeled by protonating chitosan chains using the Henderson-Hasselbalch equation. The mechanism of hydrogel network formation will be presented. The self-assembled polymer network qualitatively reproduce many experimental observables such as the pH-dependent strain-stress curve, bulk moduli, and structure factor. Our model is also capable of simulating other similar polyelectrolyte polymer systems. [Preview Abstract] |
Thursday, March 17, 2016 9:48AM - 10:24AM |
R38.00010: Bio-Inspired Metal-Coordination Dynamics: A Unique Tool for Engineering Soft Matter Mechanics Invited Speaker: Niels Holten-Andersen Growing evidence supports a critical role of metal-coordination in soft biological material properties such as self-healing, underwater adhesion and autonomous wound plugging. Using bio-inspired metal-binding polymers, initial efforts to mimic these properties with metal-coordination crosslinked polymer materials have shown promise. In addition, with polymer network mechanics strongly coupled to coordinate crosslink dynamics material properties can be easily tuned from visco-elastic fluids to solids. Given their exploitation in desirable material applications in Nature, bio-inspired metal-coordinate complex crosslinking provides an opportunity to further advance synthetic polymer materials design. Early lessons from this pursuit are presented. [Preview Abstract] |
Thursday, March 17, 2016 10:24AM - 10:36AM |
R38.00011: A Molecular Framework for Tunable Functional Response of Programmable Polyesters Kshitij C. Jha, Abraham Joy, Mesfin Tsige All-atom molecular dynamics (MD) simulations, using the OPLS force field, were carried out on a library of multifunctional polyesters with peptide-like functional pendant groups. The polyesters are structural peptidomimetics and can be utilized for applications in sensing, and separation, and as biomedical scaffolds. The modular design of the polyesters affords a range of hydrophilic and hydrophobic behavior. We used MD to quantify the hydrogen bond dynamics, end-to-end distance, and radii of gyration with changes in side group functionality, concentration, and temperature. We discerned trends for the physical behavior of polyesters with change in nature and ratio of the side groups. We also observed functional assembly for dissimilar polyesters, and correlated the assembly to the affinity of side groups. The trends in physical behavior and dissimilar assembly can be mined for iterative design towards programmatic assembly of the modular multifunctional polyesters under study. [Preview Abstract] |
Thursday, March 17, 2016 10:36AM - 10:48AM |
R38.00012: Effects of Crowder Structure and Salt on DNA Mobility and Conformation in Crowded Environments Stephanie M. Gorczyca, Rae M. Robertson-Anderson Biological cells are crowded environments in which DNA must move through to perform specific functions. We study how the properties of crowded cell-like environments impact DNA dynamics by tracking individual 115 kbp ring and linear DNA in different crowded environments using single-molecule fluorescence microscopy. We determine the role of crowder structure and salt on DNA diffusion and conformation by measuring the mean-squared center-of-mass displacements, as well as the conformational shape, size, and fluctuations of each molecule. Previously, we used 10 and 500 kDa dextran as crowders and showed that mobility of both ring and linear DNA decreased exponentially with increased crowding, but rings compact while linear DNA elongate. These effects were dependent solely on the reduction in available volume for DNA rather than size or number of crowders. Here we use crowders of similar molecular weight, but different structure to dextran (10 kDa PEG and 400 kDa Ficoll). We find that DNA mobility reduction is independent of crowder structure and that ring and linear DNA undergo more significant compaction. Finally, we characterize the role of salt on DNA mobility and conformation to determine the relative roles of enthalpic versus entropic effects on crowding-induced DNA dynamics. [Preview Abstract] |
Thursday, March 17, 2016 10:48AM - 11:00AM |
R38.00013: Altered Sputum Microstructure as a Marker of Airway Obstruction in Cystic Fibrosis Patients Gregg Duncan, James Jung, Natalie West, Michael Boyle, Jung Soo Suk, Justin Hanes In the lungs of cystic fibrosis (CF) patients, highly viscoelastic mucus remains stagnant in the lung leading to obstructed airways prone to recurrent infections. Bulk-fluid rheological measurement is primarily used to assess the pathological features of mucus. However, this approach is limited in detecting microscopic properties on the length scale of pathogens and immune cells. We have shown in prior work based on the transport of muco-inert nanoparticles (MIP) in CF sputum that patients can carry significantly different microstructural properties. In this study, we aimed to determine the factors leading to variations between patients in sputum microstructure and their clinical implications. The microrheological properties of CF sputum were measured using multi-particle tracking experiments of MIP. MIP were made by grafting polyethylene glycol onto the surface of polystyrene nanoparticles which prior work has shown prevents adhesion to CF sputum. Biochemical analyses show that sputum microstructure was significantly altered by elevated mucin and DNA content. Reduction in sputum pore size is characteristic of patients with obstructed airways as indicated by measured pulmonary function tests. Our microstructural read-out may serve as a novel biomarker for CF. [Preview Abstract] |
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