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PubMed2003

Influence of solvent quality on effective pair potentials between polymers in solution.

Solutions of interacting linear polymers are mapped onto a system of "soft" spherical particles interacting via an effective pair potential. This coarse-graining reduces the individual monomer-level description to a problem involving only the center of mass (c.m.) of the polymer coils. The effective pair potentials are derived by inverting the c.m. pair distribution function, generated in Monte Carlo simulations, using the hypernetted chain closure. The method, previously devised for the self-avoiding walk model of polymers in good solvent, is extended to the case of polymers in solvents of variable quality by adding a finite nearest-neighbor monomer-monomer attraction to the previous model and varying the temperature. The resulting effective pair potential is found to depend strongly on temperature and polymer concentration. At low concentration the effective interaction becomes increasingly attractive as the temperature decreases, eventually violating thermodynamic stability criteria. However, as polymer concentration is increased at fixed temperature, the effective interaction reverts to mostly repulsive behavior. These issues help to illustrate some fundamental difficulties encountered when coarse-graining complex systems via effective pair potentials.

Journal Article↗

PubMed2003

Conformational transitions of a semiflexible polymer in nematic solvents.

Conformations of a single semiflexible polymer chain dissolved in a low-molecular-weight liquid crystalline solvent (nematogen) are examined by using a mean field theory. We take into account a stiffness and partial orientational ordering of the polymer. As a result of an anisotropic coupling between the polymer and nematogen, we predict a discontinuous (or continuous) phase transition from a condensed-rodlike conformation to a swollen one of the polymer chain, depending on the stiffness of the polymer. We also discuss the effects of the nematic interaction between polymer segments.

Journal Article↗

PubMed2004

Isotropic-nematic phase transition in suspensions of filamentous virus and the neutral polymer Dextran.

We present an experimental study of the isotropic-nematic phase transition in an aqueous mixture of charged semiflexible rods ( fd virus) and neutral polymer (Dextran). A complete phase diagram is measured as a function of ionic strength and polymer molecular weight. At high ionic strength we find that adding polymer widens the isotropic-nematic coexistence region with polymers preferentially partitioning into the isotropic phase, while at low ionic strength the added polymer has no effect on the phase transition. The nematic order parameter is determined from birefringence measurements and is found to be independent of polymer concentration (or equivalently the strength of attraction). The experimental results are compared with the existing theoretical predictions for the isotropic-nematic transition in rods with attractive interactions.

Journal Article↗

PubMed2005

Surface forces in a confined polymer melt: self-consistent field analysis of full and restricted equilibrium cases.

In full equilibrium the self-consistent field theory for a homopolymer melt confined between two surfaces predicts pronounced oscillatory interaction forces on the monomer length scale. However, when not all the polymer molecules can reversibly equilibrate with the bulk, the trapped molecules may be squeezed, adding a repulsive contribution to the interaction energy. The classical constrained or restricted equilibrium approach by Scheutjens and Fleer two decades ago to deal with this for polymers adsorbed from dilute solutions, breaks down in semidilute and concentrated polymer solutions. We present a generalized restricted equilibrium ansatz applicable also for concentrated polymer solutions. The key idea is that only the adsorbed polymer molecules, i.e., molecules that touch the surface at least once, are forced to remain inside the gap, whereas the nonadsorbing chains are free to move out of the gap when the surfaces approach each other. As in dilute solutions, the forces found in confined melt with trapped adsorbed chains become repulsive. We analyse the dependence of the interaction forces both in full as well as in restricted equilibrium cases as a function of the chain length and the interactions with the surface for a compressible polymer melt.

Journal Article↗

PubMed2005

Dynamics of distorted cholesterics in a mesogenic versus isotropic polymer network.

The dynamics of the distorted cholesteric director is studied in a complex matrix, such as mesogenic and istotropic polymer networks, by means of dynamic light scattering. We employ polymer-stabilized cholesteric diffraction gratings as our system to measure thermal fluctuations of the cholesteric director in photostabilized low-molecular-weight polymer networks. The relaxation rates of fast and slow dynamical modes of the distorted cholesteric directors are measured in two scattering geometries, where the scattering vector is either parallel or perpendicular to the helical axis. The dispersion relations for fluctuation wave vectors along the helical axis are found to be fundamentally different for the two types of polymer networks. Experimental dispersion curves are in agreement with the theoretical predictions developed in the present paper. A possible understanding of dispersion in distorted cholesterics is developed and the experimental results for polymer stabilized cholesteric diffraction gratings are presented in this report. We also discuss the coupling of a slow relaxation mode of distorted cholesterics in a mesogenic versus isotropic polymer network.

Journal Article↗

PubMed2005

Fluctuation spectrum of membranes with anchored linear and star polymers.

The effect of linear homopolymers, diblock copolymers, and star polymers anchored to a membrane on the membrane's fluctuation spectrum is investigated for low grafting densities. Due to the nonlocality of the polymer-membrane interaction, the effective bending rigidity kappa(eff)(q) of the composite membrane is found to depend strongly on the wave vector q of the membrane undulations. Analytical calculations for ideal linear chains and simulations for ideal and self-avoiding linear chains as well as for star polymers are presented. The analytical calculations are based on the Green's function approach of Bickel and Marques [Eur. Phys. J. E 9, 349 (2002)]; for the simulations the Monte Carlo method is used. The functional form of kappa(eff)(q) differs for end-grafted chains and diblock copolymers. In general, the polymer effect is most pronounced for undulations on length scales larger than or comparable to the polymer size, and decreases rapidly for smaller undulation wavelengths. Anchored linear chains always increase kappa; anchored star polymers may increase as well as decrease kappa, depending on whether they are anchored symmetrically or asymmetrically to the membrane.

Biopolymers↗

PubMed2006

Single-polymer Brownian motor: a simulation study.

Numerical simulation is used to study a single polymer chain in a flashing ratchet potential to determine how the mechanism of this Brownian motor system is affected by the presence of internal degrees of freedom. The polymer is modeled by a freely jointed chain with N monomers in which the monomers interact via a repulsive Lennard-Jones potential and neighboring monomers on the chain are connected by finite extensible nonlinear elastic bonds. Each monomer is acted upon by a 1D asymmetric, piecewise linear potential of spatial period L comparable to the radius of gyration of the polymer. This potential is also characterized by a localization time, t(on), and by a free diffusion time, t(off). We characterize the average motor velocity as a function of L, t(off), and N to determine optimal parameter ranges, and we evaluate motor performance in terms of finite dispersion, Peclet number, rectification efficiency, stall force, and transportation of a load against a viscous drag. We find that the polymer motor performs qualitatively better than a single particle in a flashing ratchet: with increasing N, the polymer loses velocity much more slowly than expected in the absence of internal degrees of freedom, and the motor stall force increases linearly with N. To understand these cooperative aspects of motor operation, we analyze relevant Rouse modes. The experimental feasibility is analyzed and the parameters of the model are scaled to those of lambda-DNA. Finally, in the context of experimental realization, we present initial modeling results for a 2D flashing ratchet constructed using an electrode array, and find good agreement with the results of 1D simulations although the polymer in the 2D potential sometimes briefly "detaches" from the electrode surface.

Journal Article↗

PubMed2006

Dynamic scaling in entangled mean-field gelation polymers.

We present a simple reaction kinetics model to describe the polymer synthesis used by Lusignan et al. [Phys. Rev. E 60, 5657 (1999)] to produce randomly branched polymers in the vulcanization class. Numerical solution of the rate equations gives probabilities for different connections in the final product, which we use to generate a numerical ensemble of representative molecules. All structural quantities probed in the experiments are in quantitative agreement with our results for the entire range of molecular weights considered. However, with detailed topological information available in our calculations, our estimate of the "rheologically relevant" linear segment length is smaller than that estimated from the experimental results. We use a numerical method based on a tube model of polymer melts to calculate the rheological properties of such molecules. Results are in good agreement with experiment, except that in the case of the largest molecular weight samples our estimate of the zero-shear viscosity is significantly lower than the experimental findings. Using acid concentration as an indicator for closeness to the gelation transition, we show that the high-molecular-weight polymers considered are at the limit of mean-field behavior--which possibly is the reason for this disagreement. For a truly mean-field gelation class of model polymers, we numerically calculate the rheological properties for a range of segment lengths. Our calculations show that the tube theory with dynamical dilation predicts that, very close to the gelation limit, the contribution to viscosity for this class of polymers is dominated by the contribution from constraint-release Rouse motion and the final viscosity exponent approaches a Rouse-like value.

Journal Article↗

PubMed2006

Adsorption and desorption of reversible supramolecular polymers.

We report numerical mean-field results on the quasichemical level of approximation that describe adsorption of reversible supramolecular polymers at a flat interface. Emphasis is laid on the regime of strong adsorption from a dilute solution. There are two differences with respect to macromolecular polymer adsorption: (i) adsorption sets in at relatively high monomer concentrations of the surrounding solution, and (ii) the surface is filled within a much narrower concentration range. Contrary to macromolecular polymers, supramolecular polymers can therefore be desorbed by dilution of the equilibrium solution by solvent within an experimentally accessible concentration window. Based on simple thermodynamic arguments, we provide a quantitative explanation why supramolecular polymers adsorb at relatively high concentrations. Moreover, we discuss the (by comparison) narrow concentration window wherein filling of the surface occurs. This is attributed to the cooperative nature of supramolecular polymer adsorption. The degree of cooperativity is quantified by means of the Hill parameter n.

Journal Article↗

PubMed1992

Cell Wall Changes in Nectarines (Prunus persica) : Solubilization and Depolymerization of Pectic and Neutral Polymers during Ripening and in Mealy Fruit.

Nectarine fruit (Prunus persica L. Batsch var nectarina [Ait] maxim) cultivar Fantasia were either ripened immediately after harvest at 20 degrees C or stored for 5 weeks at 2 degrees C prior to ripening. Fruit ripened after 5 weeks of storage did not soften to the same extent as normally ripened fruit, they lacked juice, and had a dry, mealy texture. Pectic and hemicellulosic polysaccharides were solubilized from the mesocarp of the fruit using phenol:acetic acid:water (PAW) treatment to yield PAW-soluble material and cell wall material (CWM). The carbohydrate composition and relative molecular weight (M(r)) of polysaccharide fractions released from the CWM by sequential treatment with cyclohexane-trans-1,2-diamine tetra-acetate, 0.05 m Na(2)CO(3), 6 m guanidinium thiocyanate, and 4 m KOH were determined. Normal ripening of nectarines resulted in solubilization of pectic polymers of high M(r) from CWM during the first 2 d at ripening temperatures. Concurrently, galactan side chains were removed from pectic polymers. Solubilized pectic polymers were depolymerized to lower M(r) species during the latter stages of ripening. Upon removal from cool storage, fruit had undergone some pectic polymer solubilization, and after ripening, pectins were not depolymerized and were of high M(r). Side chains did not appear to be removed from insoluble pectic polymers and branched pectins accumulated in the CWM. The molecular weight profiles obtained by gel filtration of the hemicellulosic fractions from normally ripening and mealy fruit were similar. The results suggest that mealiness results as a consequence of altered pectic polymer breakdown, including that associated with neutral side chains.

Journal Article↗

PubMed1992

Cell Wall Dissolution in Ripening Kiwifruit (Actinidia deliciosa) : Solubilization of the Pectic Polymers.

Pectic polysaccharides solubilized in vivo during ripening, were isolated using phenol, acetic acid, and water (PAW) from the outer pericarp of kiwifruit (Actinidia deliciosa [A. Chev.] C.F. Liang and A.R. Ferguson var deliciosa ;Hayward') before and after postharvest ethylene treatment. Insoluble polysaccharides of the cell wall materials (CWMs) were solubilized in vitro by chemical extraction with 0.05 molar cyclohexane-trans-1,2-diamine tetraacetate (CDTA), 0.05 molar Na(2)CO(3), 6 molar guanidinium thiocyanate, and 4 molar KOH. The Na(2)CO(3)-soluble fraction decreased by 26%, and the CDTA-soluble fraction increased by 54% 1 day after ethylene treatment. Concomitantly, an increase in the pectic polymer content of the PAW-soluble fraction occurred without loss of galactose from the cell wall. The molecular weight of the PAW-soluble pectic fraction 1 day after ethylene treatment was similar to that of the Na(2)CO(3)-soluble fraction before ethylene treatment. Four days after ethylene treatment, 60% of cell wall polyuronide was solubilized, and 50% of the galactose was lost from the CWM, but the degree of galactosylation and molecular weight of pectic polymers remaining in the CWMs did not decrease. The exception was the CDTA-soluble fraction which showed an apparent decrease in molecular weight during ripening. Concurrently, the PAW-soluble pectic fraction showed a 20-fold reduction in molecular weight. The results suggest that considerable solubilization of the pectic polymers occurred during ripening without changes to their primary structure or degree of polymerization. Following solubilization, the polymers then became susceptible to depolymerization and degalactosidation. Pectolytic enzymes such as endopolygalacturonase and beta-galactosidase were therefore implicated in the degradation of solubilized cell wall pectic polymers but not the initial solubilization of the bulk of the pectic polymers in vivo.

Journal Article↗

PubMed1997

Microwave pressure chamber processing of a denture repair polymer.

Most denture base repairs are made using a chemically activated acrylic resin polymer for reasons of cost and expediency. Heat-activated polymers are not typically used because they require a custom split cast gypsum mold, longer polymerization time, and higher laboratory fees. Repairs made using a chemically activated polymer compared with a heat-activated polymer generally have reduced transverse strength, poorer color stability, increased water sorption, and weak bond strength to existing acrylic resin. A method of utilizing a microwave polymer in a commercially available microwave flask is described. This technique allows denture base repairs to be made with a heat-activated polymer in a manner similar to that of chemically activated repairs.

Acrylic Resins↗

PubMed1989

Glucose polymer syrup attenuates prolonged endurance exercise-induced vasopressin release.

We investigated the effect of glucose and glucose polymer ingestion on plasma arginine vasopressin (pAVP) levels, on plasma osmolality (p-osm), and on performance during two prolonged endurance events. The study subjects were 37 Finnish elite endurance athletes, of whom 18 were orienteers and 19 cross-country skiers. Plasma AVP increased in both combined glucose and glucose polymer groups, but the increase in the glucose polymer group was significantly smaller (P less than 0.001) than that in the glucose group. A significant change in p-osm caused a significant change in pAVP and vice versa. Both the orienteers and the skiers on glucose polymer tended to have more success in the competition; the orienteers on glucose polymer ran the last third of the competition significantly faster than those on glucose (P less than 0.05). It is suggested, in the light of the smaller pAVP response, that after glucose polymer ingestion the physical stress in prolonged endurance exercise is smaller than after ingestion of glucose.

Adult↗

PubMed1998

Integrated optoelectronic devices based on conjugated polymers

An all-polymer semiconductor integrated device is demonstrated with a high-mobility conjugated polymer field-effect transistor (FET) driving a polymer light-emitting diode (LED) of similar size. The FET uses regioregular poly(hexylthiophene). Its performance approaches that of inorganic amorphous silicon FETs, with field-effect mobilities of 0.05 to 0.1 square centimeters per volt second and ON-OFF current ratios of >10(6). The high mobility is attributed to the formation of extended polaron states as a result of local self-organization, in contrast to the variable-range hopping of self-localized polarons found in more disordered polymers. The FET-LED device represents a step toward all-polymer optoelectronic integrated circuits such as active-matrix polymer LED displays.

Journal Article↗

PubMed2000

Control of energy transfer in oriented conjugated polymer-mesoporous silica composites

Nanoscale architecture was used to control energy transfer in semiconducting polymers embedded in the channels of oriented, hexagonal nanoporous silica. Polarized femtosecond spectroscopies show that excitations migrate unidirectionally from aggregated, randomly oriented polymer segments outside the pores to isolated, aligned polymer chains within the pores. Energy migration along the conjugated polymer backbone occurred more slowly than Forster energy transfer between polymer chains. The different intrachain and interchain energy transfer time scales explain the behavior of conjugated polymers in a range of solution environments. The results provide insights for optimizing nanostructured materials for use in optoelectronic devices.

Journal Article↗

PubMed2002

Distribution of microbes producing antimicrobial epsilon-poly-L-lysine polymers in soil microflora determined by a novel method.

We developed a simple and sensitive screening method to investigate the distribution of microbes producing an antimicrobial poly(amino acid), epsilon-poly-L-lysine (epsilon-PL), in microflora. An acidic dye, Poly R-478, incorporated in an agar plate detected epsilon-PL producers by electrostatic interaction with the secreted basic polymers. All epsilon-PL producers, isolated after careful and sufficient screening of soil microflora, belonged exclusively to two groups of bacteria of the family Streptomycetaceae and ergot fungi. They were characterized based on the density and diameter of the concentric zone formed by the secreted polymers. The density depended on each isolate. The increase in the diameter of the concentric zone per unit of time varied among isolates and was negatively correlated with the molecular weight. Although the distribution of epsilon-PL producers was extremely limited, their products were structurally varied. The molecular masses of the secreted polymers among the isolates ranged from 0.8 to 2.0 kDa. There were also isolates producing unknown polymers inconsistent with the correlation or producing a mixture of polymers with original and modified structures. A chemically modified polymer was an epsilon-PL derivative, as determined by mass spectrometry. Since the structural variations had no relation to the phylogenetic position of the isolates, it is possible that enzymes involved in the synthesis diversified after putative horizontal transfers of relevant genes.

Bacteria↗

PubMed2000

Involvement of CD14 and beta2-integrins in activating cells with soluble and particulate lipopolysaccharides and mannuronic acid polymers.

Lipopolysaccharide (LPS) and related bacterial products can be recognized by host inflammatory cells in a particulate, bacterium-bound form, as well as in various soluble, released forms. In the present study we have compared the mechanisms used by LPS, detoxified LPS (DLPS), and mannuronic acid polymers (M-polymers), in solution or covalently linked to particles, in stimulating monocytes to tumor necrosis factor (TNF) production. The addition of recombinant LPS binding protein (LBP) and/or soluble CD14 (sCD14) enhanced the production of TNF from monocytes stimulated with soluble LPS, DLPS, or M-polymer, but did not affect the response to M-polymer or DLPS attached to particles. Treatment of monocytes with antibody to CD14, CD18, or CD11b showed that CD14, but not CR3 (CD11b/CD18), mediated monocyte TNF production in response to the soluble antigens. In contrast, anti-CD14, anti-CD11b and anti-CD18 monoclonal antibodies all inhibited the response to the particulate stimuli. On the other hand, B975, a synthetic analog of Rhodobacter capsulatus lipid A, completely abrogated the monocyte TNF response induced by LPS but did not affect the TNF induction by DLPS or M-polymer, either in soluble or particulate forms. These data demonstrate that the engagement of immune receptors by bacterial products such as LPS, DLPS, and M-polymer is dependent upon the presentation form of their constituent carbohydrates, and that factors such as aggregation state, acylation, carbohydrate chain length, and solid versus liquid phase of bacterial ligands influence the mechanisms used by cells in mediating proinflammatory responses.

Acute-Phase Proteins↗

PubMed2004

The Polymeal: a more natural, safer, and probably tastier (than the Polypill) strategy to reduce cardiovascular disease by more than 75%.

OBJECTIVE: Although the Polypill concept (proposed in 2003) is promising in terms of benefits for cardiovascular risk management, the potential costs and adverse effects are its main pitfalls. The objective of this study was to identify a tastier and safer alternative to the Polypill: the Polymeal. METHODS: Data on the ingredients of the Polymeal were taken from the literature. The evidence based recipe included wine, fish, dark chocolate, fruits, vegetables, garlic, and almonds. Data from the Framingham heart study and the Framingham offspring study were used to build life tables to model the benefits of the Polymeal in the general population from age 50, assuming multiplicative correlations. RESULTS: Combining the ingredients of the Polymeal would reduce cardiovascular disease events by 76%. For men, taking the Polymeal daily represented an increase in total life expectancy of 6.6 years, an increase in life expectancy free from cardiovascular disease of 9.0 years, and a decrease in life expectancy with cardiovascular disease of 2.4 years. The corresponding differences for women were 4.8, 8.1, and 3.3 years. CONCLUSION: The Polymeal promises to be an effective, non-pharmacological, safe, cheap, and tasty alternative to reduce cardiovascular morbidity and increase life expectancy in the general population.

Cacao↗