arXiv subjects

Roland R. Netz

Publications and source records attributed to Roland R. Netz.

At least 109 records · Page 6Linked to original sources

arXiv2008

Discrete elastic model for stretching-induced flagellar polymorphs

Force-induced reversible transformations between coiled and normal polymorphs of bacterial flagella have been observed in recent optical-tweezer experiment. We introduce a discrete elastic rod model with two competing helical states governed by a fluctuating spin-like variable that represents the underlying conformational states of flagellin monomers. Using hybrid Brownian dynamics Monte-Carlo simulations, we show that a helix undergoes shape transitions dominated by domain wall nucleation and motion in response to externally applied uniaxial tension. A scaling argument for the critical force is presented in good agreement with experimental and simulation results. Stretching rate-dependent elasticity including a buckling instability are found, also consistent with the experiment.

cond-mat.soft↗

arXiv2008

Stretching helical nano-springs at finite temperature

Using dynamic simulations and analytic methods, we study the elastic response of a helical filament subject to uniaxial tension over a wide range of bend and twist persistence length. A low-pitch helix at low temperatures exhibits a stretching instability and the force-extension curve consists of a sequence of spikes. At elevated temperature (i.e. small persistence lengths) the helix melts and a pronounced force plateau is obtained in the fixed-extension ensemble. The torque boundary condition significantly affects the resulting elastic properties.

cond-mat.soft↗

arXiv2008

Non-equilibrium hydrodynamics of a rotating filament

The nonlinear dynamics of an elastic filament that is forced to rotate at its base is studied by hydrodynamic simulation techniques; coupling between stretch, bend, twist elasticity and thermal fluctuations is included. The twirling-overwhirling transition is located and found to be strongly discontinuous. For finite bend and twist persistence length, thermal fluctuations lower the threshold rotational frequency, for infinite persistence length the threshold agrees with previous analytical predictions.

cond-mat.soft↗

arXiv2006

Ground state structure and interactions between dimeric 2D Wigner crystals

We study the ground state ordering and interactions between two two-dimensional Wigner crystals on neutralizing charged plates by means of computer simulation. We consider crystals formed by (i) point-like charges and (ii) charged dimers, which mimic the screening of charged surfaces by elongated multivalent ions such as aspherical globular proteins, charged dendrimers or short stiff polyelectrolytes. Both systems, with point-like and dimeric ions, display five distinct crystalline phases on increasing the interlayer distance. In addition to alteration of translational ordering within the bilayer, the phase transitions in the dimeric system are characterized by alteration of orientational ordering of the ions.

cond-mat.soft↗

arXiv2006

Propulsion with a Rotating Elastic Nanorod

The dynamics of a rotating elastic filament is investigated using Stokesian simulations. The filament, straight and tilted with respect to its rotation axis for small driving torques, undergoes at a critical torque a strongly discontinuous shape bifurcation to a helical state. It induces a substantial forward propulsion whatever the sense of rotation: a nanomechanical force-rectification device is established.

cond-mat.soft↗

arXiv2005

Pulling adsorbed polymers from surfaces with the AFM: stick versus slip, peeling versus gliding

We consider the response of an adsorbed polymer that is pulled by an AFM within a simple geometric framework. We separately consider the cases of i) fixed polymer-surface contact point, ii) sticky case where the polymer is peeled off from the substrate, and iii) slippery case where the polymer glides over the surface. The resultant behavior depends on the value of the surface friction coefficient and the adsorption strength. Our resultant force profiles in principle allow to extract both from non-equilibrium force-spectroscopic data.

cond-mat.soft↗

arXiv2005

Theoretical Approaches to Neutral and Charged Polymer Brushes

Neutral or charged polymers that are densely end-grafted to surfaces form brush-like structures and are highly stretched under good-solvent conditions. We discuss and compare relevant results from scaling models, self-consistent-field methods and MD simulation techniques and concentrate on the conceptual simple case of planar substrates. For neutral polymers the main quantity of interest is the brush height and the polymer density profile, which can be well predicted from self-consistent calculations and simulations. Charged polymers (polyelectrolytes) are of practical importance since they are soluble in water. Counterion degrees of freedom determine the brush behavior in a decisive way and lead to a strong and non-linear swelling of the brush.

cond-mat.soft↗

arXiv2005

Electrostatic Interactions in Strongly-Coupled Soft Matter

Charged soft-matter systems--such as colloidal dispersions and charged polymers--are dominated by attractive forces between constituent like-charged particles when neutralizing counterions of high charge valency are introduced. Such counter-intuitive effects indicate strong electrostatic coupling between like-charged particles, which essentially results from electrostatic correlations among counterions residing near particle surfaces. In this paper, the attraction mechanism and the structure of counterionic correlations are discussed in the limit of strong coupling based on recent numerical and analytical investigations and for various geometries (planar, spherical and cylindrical) of charged objects.

cond-mat.soft↗

arXiv2005

Scaling and Universality in the Counterion-Condensation Transition at Charged Cylinders

We address the critical and universal aspects of counterion-condensation transition at a single charged cylinder in both two and three spatial dimensions using numerical and analytical methods. By introducing a novel Monte-Carlo sampling method in logarithmic radial scale, we are able to numerically simulate the critical limit of infinite system size (corresponding to infinite-dilution limit) within tractable equilibration times. The critical exponents are determined for the inverse moments of the counterionic density profile (which play the role of the order parameters and represent the inverse localization length of counterions) both within mean-field theory and within Monte-Carlo simulations. In three dimensions (3D), correlation effects (neglected within mean-field theory) lead to an excessive accumulation of counterions near the charged cylinder below the critical temperature (condensation phase), while surprisingly, the critical region exhibits universal critical exponents in accord with the mean-field theory. In two dimensions (2D), we demonstrate, using both numerical and analytical approaches, that the mean-field theory becomes exact at all temperatures (Manning parameters), when number of counterions tends to infinity. For finite particle number, however, the 2D problem displays a series of peculiar singular points (with diverging heat capacity), which reflect successive de-localization events of individual counterions from the central cylinder. In both 2D and 3D, the heat capacity shows a universal jump at the critical point, and the energy develops a pronounced peak. The asymptotic behavior of the energy peak location is used to locate the critical temperature, which is also found to be universal and in accordance with the mean-field prediction.

cond-mat.soft↗

arXiv2005

Non-linear Osmotic Brush Regime: Simulations and mean-field theory

We investigate polyelectrolyte brushes in the osmotic regime using both theoretical analysis and molecular dynamics simulation techniques. In the simulations at moderate Bjerrum length, we observe that the brush height varies weakly with grafting density, in contrast to the accepted scaling law, which predicts a brush thickness independent of the grafting density. We show that such behavior can be explained by considering lateral electrostatic effects (within the non-linear Poisson-Boltzmann theory) combined with the coupling between lateral and longitudinal degrees of freedom due to the conserved polymer volume (which are neglected in scaling arguments). We also take the non-linear elasticity of polyelectrolyte chains into consideration, which makes significant effects as chains are almost fully stretched in the osmotic regime. It is shown that all these factors lead to a non-monotonic behavior for the brush height as a function of the grafting density. At large grafting densities, the brush height increases with increasing the grafting density due to the volume constraint. At small grafting densities, we obtain a re-stretching of the chains for decreasing grafting density, which is caused by lateral electrostatic contributions and the counterion-condensation process at polyelectrolyte chains. These results are obtained assuming all counterions to be trapped within the brush, which is valid for sufficiently long chains of large charge fraction.

cond-mat.soft↗

arXiv2005

Attraction of like-charged macroions in the strong-coupling limit

Like-charged macroions attract each other as a result of strong electrostatic correlations in the presence of multivalent counterions or at low temperatures. We investigate the effective electrostatic interaction between i) two like-charged rods and ii) two like-charged spheres using the recently introduced strong-coupling theory, which becomes asymptotically exact in the limit of large coupling parameter (i.e. for large counterion valency, low temperature, or high surface charge density on macroions). Since we deal with curved surfaces, an additional parameter, referred to as Manning parameter, is introduced, which measures the ratio between the radius of curvature of macroions to the Gouy-Chapman length and controls the counterion-condensation process that directly affects the effective interactions. For sufficiently large Manning parameters (weakly-curved surfaces), we find a strong long-ranged attraction between two macroions that form a closely-packed bound state with small surface-to-surface separation of the order of the counterion diameter in agreement with recent simulations. For small Manning parameters (highly-curved surfaces), on the other hand, the equilibrium separation increases and the macroions unbind from each other as the confinement volume increases to infinity. This occurs via a continuous universal unbinding transition for two charged rods at a threshold Manning parameter of 2/3, while the transition is discontinuous for spheres because of a pronounced potential barrier at intermediate distances.

cond-mat.soft↗

arXiv2005

Non-linear Osmotic Brush Regime: Experiments, Simulations and Scaling Theory

We experimentally and theoretically consider highly condensed planar brushes made of charged polymers. Using x-ray reflectivity on polyelectrolytes which are anchored at the water-air interface, it is shown that such strongly stretched brushes show a slight but detectable height variation upon lateral compression. This stands in contrast to the well-accepted scaling relation in the so-called osmotic brush regime, which predicts the brush height to be independent of the grafting density. Similar effects are seen in simulations on highly compressed charged brushes. Scaling arguments which go beyond the linear approximation for the entropy of confined counterions and for weak chain-stretching are able to explain those findings on a semi-quantitative level.

cond-mat.soft↗

arXiv2005

Counterions at Charged Cylinders: Criticality and universality beyond mean-field

The counterion-condensation transition at charged cylinders is studied using Monte-Carlo simulation methods. Employing logarithmically rescaled radial coordinates, large system sizes are tractable and the critical behavior is determined by a combined finite-size and finite-ion-number analysis. Critical counterion localization exponents are introduced and found to be in accord with mean-field theory both in 2 and 3 dimensions. In 3D the heat capacity shows a universal jump at the transition, while in 2D, it consists of discrete peaks where single counterions successively condense.

cond-mat.soft↗

arXiv2005

Attraction and unbinding of like-charged rods

We investigate the effective interaction between two like-charged rods in the regime of large electrostatic coupling parameters using both Molecular Dynamics simulation techniques and the recently introduced strong-coupling theory. We obtain attraction between the rods for elevated Manning parameters accompanied by an equilibrium surface-to-surface separation of the order of the Gouy-Chapman length. A continuous unbinding between the rods is predicted at a threshold Manning parameter of 2/3.

cond-mat.soft↗

arXiv2004

Variational theory for a single polyelectrolyte chain revisited

We reconsider the electrostatic contribution to the persistence length, $\ell_e$, of a single, infinitely long charged polymer in the presence of screening. A Gaussian variational method is employed, taking $\ell_e$ as the only variational parameter. For weakly charged and flexible chains, crumpling occurs at small length scales because conformational fluctuations overcome electrostatic repulsion. The electrostatic persistence length depends on the square of the screening length, $\ell_e\simκ^{-2}$, as first argued by Khokhlov and Khachaturian by applying the Odijk-Skolnick-Fixman (OSF) theory to a string of crumpled blobs. We compare our approach to previous theoretical works (including variational formulations) and show that the result $\ell_e\simκ^{-1}$ found by several authors comes from the improper use of a cutoff at small length scales. For highly charged and stiff chains, crumpling does not occur; here we recover the OSF result and validate the perturbative calculation for slightly bent rods.

cond-mat.soft↗

arXiv2003

Electrostatic colloid-membrane complexation

We investigate numerically and on the scaling level the adsorption of a charged colloid on an oppositely charged flexible membrane. We show that the long ranged character of the electrostatic interaction leads to a wrapping reentrance of the complex as the salt concentration is varied. The membrane wrapping depends on the size of the colloid and on the salt concentration and only for intermediate salt concentration and colloid sizes we find full wrapping. From the scaling model we derive simple relations for the phase boundaries between the different states of the complex, which agree well with the numerical minimization of the free energy.

physics.bio-ph↗

arXiv2002

Variational charge renormalization in charged systems

We apply general variational techniques to the problem of the counterion distribution around highly charged objects where strong condensation of counterions takes place. Within a field-theoretic formulation using a fluctuating electrostatic potential, the concept of surface-charge renormalization is recovered within a simple one-parameter variational procedure. As a test, we reproduce the Poisson-Boltzmann surface potential for a single charge planar surface both in the weak-charge and strong-charge regime. We then apply our techniques to non-planar geometries where closed-form solutions of the non-linear Poisson-Boltzmann equation are not available. In the cylindrical case, the Manning charge renormalization result is obtained in the limit of vanishing salt concentration. However, for intermediate salt concentrations a slow crossover to the non-charge-renormalized regime (at high salt) is found with a quasi-power-law behavior which helps to understand conflicting experimental and theoretical results for the electrostatic persistence length of polyelectrolytes. In the spherical geometry charge renormalization is only found at intermediate salt concentrations.

cond-mat.soft↗

arXiv2002

Systematic Field-Theory for the Hard-Core One-Component Plasma

An accurate and systematic equation of state for the hard-core one-component plasma (HCOCP) is obtained. The result is based on the Hubbard-Schofield transformation which yields the field-theoretical Hamiltonian, with coefficients expressed in terms of equilibrium correlation functions of the reference hard-core fluid. Explicit calculations were performed using the Gaussian approximation for the effective Hamiltonian and known thermodynamic and structural properties of the reference hard-core fluid. For small values of the plasma parameter G and packing fraction the Debye-Huckel result is recovered, while for G>>1, the excess free energy F_ex and internal U_{ex} energy depend linearly on G. The obtained expression for U_ex is in a good agreement with the available Monte Carlo data for the HCOCP. We also analyse the validity of the widely used approximation, which represents the free energy as a sum of the hard-core and electrostatic part.

cond-mat.soft↗