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Équipe "Théorie et Simulation des Polymères" (ETSP)
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Long range correlations in semidilute solutions and melts

Outline

  1. Background: Flory's ideality hypothesis for three dimensional bulks
  2. Recent results: Intra chain correlations
  3. Polymer melts in ultrathin slits: Silberberg's hypot
  4. Fluctuation-induced long-range interactions in composite polymer systems
  5. Collaboration
  6. Related papers

1. Background: Flory's ideality hypothesis for three dimensional bulks

It is commonly accepted that in concentrated solutions or melts high-molecular weight polymers display random-walk conformational properties without long range memory between subsequent bonds [1]. This has been anticipated already in the 1950s by Flory in his famous "ideality hypothesis". The absence of memory means that the correlation function, P(s), of two bonds separated by s monomers along the chain should exponentially decay with s. This is the standard basis for defining an important experimental measure of chain stiffness, the persistence length.

2. Recent results: Intra chain correlations

In our recent paper [1] we present numerical results and theoretical arguments, demonstrating a non-exponential, long ranged decay of the bond-bond correlation function P(s) as a function of the contour distance s. Suggesting a profound analogy with the well-known long range velocity correlations in liquids we find P(s) to decay algebraically as s-3/2. See the figure on the right.

As a consequence, the operational definition of the persistent length should be carefully revisited.

We have analysed in detail the polymer form factor F(q) and the total structure factor S(q) in order to provide experimental testing beds for our theoretical predicitions. For instance, we show a strinking hump in the Kratky plot representation of q2 F(q) which may be visible in neutron scattering experiments of long flexible polymers.

3. Polymer melts in ultrathin slits: Silberberg's hypothesis put to a test

Consistently, we find P(s) ~ 1/s for polymer melts in ultrathin quasi two dimensional slits [2]. The confinement has a pronounced effect on intra- and intermolecular correlations: the walls force a chain to fold back into volume it pervades; this volume is thus gradually depleted of other chains as the film thickness decreases.

The resulting reduction of chain interdigitation entails deviations from ideal behavior (Silberberg's hypothesis). We study these deviations by discussing mainly conformational properties (chain extension, intrachain structure factor, etc.) of the polymer films. Our simulation results are compared with a recent theoretical approach attempting to go beyond Silberberg's hypothesis.

4. Fluctuation-induced long-range interactions in composite polymer systems

We also challenge the applicability of the so-called "Random Phase Approximation" (A.N. Semenov and A. Johner [3]) for dense polymers. There are fluctuation-induced universal long-range forces which have the important consequence to counterbalance attractive van-der Waals forces between two colloidal particles (of size much smaller than that of a polymer coil). This should lead to a stabilization of the dispersed particles in a polymer matrix consisting of long chains. We propose to further explore this stabilization mechanism theoretically and via computer simulations. A.N. Semenov and S. Obukhov have also developed a theoretical approach predicting polymer-induced repulsion between colloidal particles in semidilute solutions [4,5]. Finding the optimal conditions for such polymer-induced colloidal stabilization is another important goal inviting theoretical investigations of the effects of concentration, molecular weight, molecular weight distribution, solvent quality, macromolecular architecture (linear, branched or other), block-copolymer structure and polymer-colloid interactions on the long-range forces.

5. Collaboration

J.P. Wittmer (principal investigator), H. Meyer, J. Baschnagel, A. Johner, A.N. Semenov, S. Obukhov (Gainesville, USA), M. Müller (Göttingen, Germany)

6. Related papers

  1. [WMBJOMMS04] J.P. Wittmer, H. Meyer, J. Baschnagel,
    A. Johner, S. Obukhov, L. Mattioni, M. Müller, A.N. Semenov
    Long Range Bond-Bond Correlations in Dense Polymer Solutions
    PRL, 93, 147801 (2004); cond-mat/0404457.

  2. [CMWJB05] A. Cavallo, M. Mueller, J.P. Wittmer, A. Johner, K. Binder
    Single chain structure in thin polymer films:
    Corrections to Flory's and Silberberg's hypotheses

    J.Phys.: Condens. Matter, 17 (25 May 2005) 1697-1709; cond-mat/0412373.

  3. [SJ03] A. N. Semenov, A. Johner
    Theoretical notes on dense polymers in two dimensions
    Eur. Phys. J. E 12, 469 (2003).

  4. [SO05] A.N. Semenov, S.P. Obukhov
    Fluctuation-induced long-range interactions in polymer systems
    J.Phys.: Condens. Matter, 17 (25 May 2005) 1747-1777.

  5. [OS05] S. P. Obukhov, A. N. Semenov
    Long-Range Interactions in Polymer Melts: The Anti-Casimir Effect
    Phys. Rev. Lett. 95, 038305 (2005).

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