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M. Ullner

Publications and source records attributed to M. Ullner.

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The Electrostatic Persistence Length Calculated from Monte Carlo, Variational and Perturbation Methods

Monte Carlo simulations and variational calculations using a Gaussian ansatz are applied to a model consisting of a flexible linear polyelectrolyte chain as well as to an intrinsically stiff chain with up to 1000 charged monomers. Addition of salt is treated implicitly through a screened Coulomb potential for the electrostatic interactions. For the flexible model the electrostatic persistence length shows roughly three regimes in its dependence on the Debye-Hückel screening length, $κ^{-1}$.As long as the salt content is low and $κ^{-1}$ is longer than the end-to-end distance, the electrostatic persistence length varies only slowly with $κ^{-1}$. Decreasing the screening length, a controversial region is entered. We find that the electrostatic persistence length scales as $sqrt{ξ_p}/κ$, in agreement with experiment on flexible polyelectrolytes, where $ξ_p$ is a strength parameter measuring the electrostatic interactions within the polyelectrolyte. For screening lengths much shorter than the bond length, the $κ^{-1}$ dependence becomes quadratic in the variational calculation. The simulations suffer from numerical problems in this regime, but seem to give a relationship half-way between linear and quadratic. A low temperature expansion only reproduces the first regime and a high temperature expansion, which treats the electrostatic interactions as a perturbation to a Gaussian chain, gives a quadratic dependence on the Debye length. For a sufficiently stiff chain, the persistence length varies quadratically with $κ^{-1}$ in agreement with earlier theories.

cond-mat.soft

Titrating Polyelectrolytes - Variational Calculations and Monte Carlo Simulations

Variational methods are used to calculate structural and thermodynamical properties of a titrating polyelectrolyte in a discrete representation. The Coulomb interactions are emulated by harmonic repulsive forces, the force constants being used as variational parameters to minimize the free energy. For the titrating charges, a mean field approach is used. The accuracy is tested against Monte Carlo data for up to 1000 monomers. For an unscreened chain, excellent agreement is obtained for the end-to-end distance and the apparent dissociation constant. With screening, the thermodynamical properties are invariably well described, although the structural agreement deteriorates. A very simple rigid-rod approximation is also considered, giving surprisingly good results for certain properties.

chem-ph