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Register a new userLocal entropic effects of polymers grafted to soft interfaces
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In this paper, we study the equilibrium properties of polymer chains end-tethered to a fluid membrane. The loss of conformational entropy of the polymer results in an inhomogeneous pressure field that we calculate for gaussian chains. We estimate the effects of excluded volume through a relation between pressure and concentration. Under the polymer pressure, a soft surface will deform. We calculate the deformation profile for a fluid membrane and show that close to the grafting point, this profile assumes a cone-like shape, independently of the boundary conditions. Interactions between different polymers are also mediated by the membrane deformation. This pair-additive potential is attractive for chains grafted on the same side of the membrane and repulsive otherwise.
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The statistical mechanics of polymers grafted on surfaces has been the subject of intense research activity because of many potential applications. In this paper, we analytically investigate the conformational changes caused by a single cross-link on two ideal (Gaussian) chains grafted on a rigid planar surface. Both the cross-link and the surface reduce the number of allowed configurations. In the absence of the hard substrate, the sole effect of the cross-link is a reduction in the effective Kuhn length of a tethered chain. The cross-link induced shrinkage (collapse) of the grafted chains (mushrooms) turns out to be a reduction in the variance of the distribution of the height of the chain rather than a reduction of the height itself.
We report Monte Carlo simulations of the self-assembly of supramolecular polymers based on a model of patchy particles. We find a first-order phase transition, characterized by hysteresis and nucleation, toward a solid bundle of polymers, of length much greater than the average gas phase length. We argue that the bundling transition is the supramolecular equivalent of the sublimation transition, that results from a weak chain-chain interaction. We provide a qualitative equation of state that gives physical insight beyond the specific values of the parameters used in our simulations.
We present the results of analytic calculations and numerical simulations of the behaviour of a new class of chain molecules which we call thick polymers. The concept of the thickness of such a polymer, viewed as a tube, is encapsulated by a special three body interaction and impacts on the behaviour both locally and non-locally. When thick polymers undergo compaction due to an attractive self-interaction, we find a new type of phase transition between a compact phase and a swollen phase at zero temperature on increasing the thickness. In the vicinity of this transition, short tubes form space filling helices and sheets as observed in protein native state structures. Upon increasing the chain length, or the number of chains, we numerically find a crossover from secondary structure motifs to a quite distinct class of structures akin to the semi-crystalline phase of polymers or amyloid fibers in polypeptides.
Binary mixtures of semiflexible polymers with the same chain length but different persistence lengths separate into two coexisting different nematic phases when the osmotic pressure of the lyotropic solution is varied. Molecular Dynamics simulations and Density Functional Theory predict phase diagrams either with a triple point, where the isotropic phase coexists with two nematic phases, or a critical point of unmixing within the nematic mixture. The difference in locally preferred bond angles between the constituents drives this unmixing without any attractive interactions between monomers.
Recent experimental developments showed that the use of the radiation pressure, induced by a continuous laser wave, to control fluid-fluid interface deformations at the microscale, represents a very promising alternative to electric or magnetic actuation. In this article, we solve numerically the dynamics and steady state of the fluid interface under the effects of buoyancy, capillarity, optical radiation pressure and viscous stress. A precise quantitative validation is shown by comparison with experimental data. New results due to the nonlinear dependence of the optical pressure on the angle of incidence are presented, showing different morphologies of the deformed interface going from needle-like to finger-like shapes, depending on the refractive index contrast. In the transient regime, we show that the viscosity ratio influences the time taken for the deformation to reach steady state.
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