arXiv subjects

C. Holm

Publications and source records attributed to C. Holm.

18 recordsLinked to original sources

arXiv2014

Effective potentials between gold nano crystals -- functional dependence on the temperature

A method is presented that allows to combine the effective potential between two nano crystals, the potential of mean force (PMF), as obtained from all-atomistic Molecular Dynamics simulations with perturbation theory. In this way, a functional dependence of the PMF on temperature is derived, that enables the prediction of the PMF in a wide temperature range. We applied the method for systems of capped gold nano crystals of different size. They show very good agreement with data from atomistic simulations.

cond-mat.soft↗

arXiv2011

2D versus 3D Freezing of a Lennard-Jones Fluid in a Slit Pore

We present a computer simulation study of a (6,12)-Lennard-Jones fluid confined to a slit pore, formed by two uniform planes. These interact via a (3,9)-Lennard-Jones potential with the fluid particles. When the fluid approaches the liquid-to-solid transition we first observe layering parallel to the walls. In order to investigate the nature of the freezing transition, we performed a detailed analysis of the bond-orientational order parameter in the layers. Changing the distance between the slit wall, we studied howthe behaviour changes from a quasi-2d crystallization without hysteresis and an intermediate hexatic phase to a standard 3d nucleation.

cond-mat.soft↗

arXiv2011

How Close to Two Dimensions Does a Lennard-Jones System Need to Be to Produce a Hexatic Phase?

We report on a computer simulation study of a Lennard-Jones liquid confined in a narrow slit pore with tunable attractive walls. In order to investigate how freezing in this system occurs, we perform an analysis using different order parameters. Although some of the parameters indicate that the system goes through a hexatic phase, other parameters do not. This shows that to be certain whether a system has a hexatic phase, one needs to study not only a large system, but also several order parameters to check all necessary properties. We find that the Binder cumulant is the most reliable one to prove the existence of a hexatic phase. We observe an intermediate hexatic phase only in a monolayer of particles confined such that the fluctuations in the positions perpendicular to the walls are less then 0.15 particle diameters, i. e. if the system is practically perfectly 2d.

cond-mat.soft↗

arXiv2009

Ensemble Inequivalence in Single Molecule Experiments

In bulk systems the calculation of the main thermodynamic quantities leads to the same expectation values in the thermodynamic limit, regardless of the choice of the statistical ensemble. Single linear molecules can be still regarded as statistical systems, where the thermodynamic limit is represented by infinitely long chains. The question of equivalence between different ensembles is not at all obvious and has been addressed in the literature, with sometimes contradicting conclusions. We address this problem by studying the scaling properties of the ensemble difference for two different chain models, as a function of the degree of polymerization. By characterizing the scaling behavior of the difference between the isotensional (Gibbs) and isometric (Helmholtz) ensembles in the transition from the low-stretching to the high-stretching regime, we show that ensemble equivalence cannot be reached for macroscopic chains in the low force regime, and we characterize the transition from the inequivalence to the equivalence regime.

cond-mat.soft↗

arXiv2009

2D versus 3D Freezing of a Lennard-Jones Fluid in a Slit Pore: A Molecular Dynamics Study

We present a computer simulation study of a (6,12)-Lennard-Jones fluid confined to a slit pore, formed by two uniform planes. These interact via (3,9)-Lennard-Jones potential with the fluid particles. When the fluid approaches the liquid-to-solid transition we first observe layering parallel to the walls. In order to investigate the nature of the freezing transition we performed a detailed analysis of the bond-orientational order parameter in the layers. We found no signs of hexatic order which would indicate a melting scenario of the Kosterlitz-Thouless type. An analysis of the mean-square displacement shows that the particles can easily move between the layers, making the crystallization a 3d-like process. This is consistent with the fact that we observe a considerable hysteresis in the heating-freezing curves, showing that the crystallization transition proceeds as an activated process.

cond-mat.soft↗

arXiv2008

P3M algorithm for dipolar interactions

An extension to the P3M algorithm for electrostatic interactions is presented, that allows to efficiently compute dipolar interactions in periodic boundary conditions. Theoretical estimates for the root-mean square error of the forces, torques and the energy are derived. The applicability of the estimates is tested and confirmed in several numerical examples. A comparison of the computational performance of the new algorithm to state-of-the-art dipolar Ewald summation methods shows a performance crossover from the Ewald method to the dipolar P3M method for as few as 300 dipolar particles. In larger systems, the new algorithm represents a substantial improvement in performance with respect to the dipolar standard Ewald method.

physics.comp-ph↗

arXiv2008

Colloidal electrophoresis: Scaling analysis, Green-Kubo relation, and numerical results

We consider electrophoresis of a single charged colloidal particle in a finite box with periodic boundary conditions, where added counterions and salt ions ensure charge neutrality. A systematic rescaling of the electrokinetic equations allows us to identify a minimum set of suitable dimensionless parameters, which, within this theoretical framework, determine the reduced electrophoretic mobility. It turns out that the salt-free case can, on the Mean Field level, be described in terms of just three parameters. A fourth parameter, which had previously been identified on the basis of straightforward dimensional analysis, can only be important beyond Mean Field. More complicated behavior is expected to arise when further ionic species are added. However, for a certain parameter regime, we can demonstrate that the salt-free case can be mapped onto a corresponding system containing additional salt. The Green-Kubo formula for the electrophoretic mobility is derived, and its usefulness demonstrated by simulation data. Finally, we report on finite-element solutions of the electrokinetic equations, using the commercial software package COMSOL.

cond-mat.soft↗

arXiv2005

Incorporation of excluded volume correlations into Poisson-Boltzmann theory

We investigate the effect of excluded volume interactions on the electrolyte distribution around a charged macroion. First, we introduce a criterion for determining when hard-core effects should be taken into account beyond standard mean field Poisson-Boltzmann (PB) theory. Next, we demonstrate that several commonly proposed local density functional approaches for excluded volume interactions cannot be used for this purpose. Instead, we employ a non-local excess free energy by using a simple constant weight approach. We compare the ion distribution and osmotic pressure predicted by this theory with Monte Carlo simulations. They agree very well for weakly developed correlations and give the correct layering effect for stronger ones. In all investigated cases our simple weighted density theory yields more realistic results than the standard PB approach, whereas all local density theories do not improve on the PB density profiles but on the contrary, deviate even more from the simulation results.

cond-mat.soft↗

arXiv2004

Magnetization of polydisperse colloidal ferrofluids: Effect of magnetostriction

We exploit magnetostriction in polydisperse ferrofluids in order to generate nonlinear responses, and apply a thermodynamical method to derive the desired nonlinear magnetic susceptibility. For an ideal gas, this method has been demonstrated to be in excellent agreement with a statistical method. In the presence of a sinusoidal ac magnetic field, the magnetization of the polydisperse ferrofluid contains higher-order harmonics, which can be extracted analytically by using a perturbation approach. We find that the harmonics are sensitive to the particle distribution and the degree of field-induced anisotropy of the system. In addition, we find that the magnetization is higher in the polydisperse system than in the monodisperse one, as also found by a recent Monte Carlo simulation. Thus, it seems possible to detect the size distribution in a polydisperse ferrofluid by measuring the harmonics of the magnetization under the influence of magnetostriction.

cond-mat.soft↗

arXiv2003

Polyelectrolyte Bundles

Using extensive Molecular Dynamics simulations we study the behavior of polyelectrolytes with hydrophobic side chains, which are known to form cylindrical micelles in aqueous solution. We investigate the stability of such bundles with respect to hydrophobicity, the strength of the electrostatic interaction, and the bundle size. We show that for the parameter range relevant for sulfonated poly-para-phenylenes (PPP) one finds a stable finite bundle size. In a more generic model we also show the influence of the length of the precursor oligomer on the stability of the bundles. We also point out that our model has close similarities to DNA solutions with added condensing agents, hinting to the possibility that the size of DNA aggregates is under certain circumstances thermodynamically limited.

cond-mat.soft↗

arXiv2003

Single chain properties of polyelectrolytes in poor solvent

Using molecular dynamics simulations we study the behavior of a dilute solution of strongly charged polyelectrolytes in poor solvents, where we take counterions explicitly into account. We focus on the chain conformational properties under conditions where chain-chain interactions can be neglected, but the counterion concentration remains finite. We investigate the conformations with regard to the parameters chain length, Coulomb interaction strength, and solvent quality, and explore in which regime the competition between short range hydrophobic interactions and long range Coulomb interactions leads to pearl-necklace like structures. We observe that large number and size fluctuations in the pearls and strings lead to only small direct signatures in experimental observables like the single chain form factor. Furthermore we do not observe the predicted first order collapse of the necklace into a globular structure when counterion condensation sets in. We will also show that the pearl-necklace regime is rather small for strongly charged polyelectrolytes at finite densities. Even small changes in the charge fraction of the chain can have a large impact on the conformation due to the delicate interplay between counterion distribution and chain conformation.

cond-mat.soft↗

arXiv2002

Computer Simulations of charged systems

In this brief contribution to the Proceedings of the NATO-ASI on ``Electrostatic Effects in Soft Matter and Biophysics'', which took place in Les Houches from Oct. 1-13, 2000, we summarize in short aspects of the simulations methods to study charged systems. After describing some basics of Monte Carlo and Molecular dynamics techniques, we describe a few methods to compute long range interactions in periodic systems. After a brief detour to mean-field models, we describe our results obtained for flexible polyelectrolytes in good and bad solvents. We follow with a description of the inhomogeneity of the counterion distribution around finite chains, and continue then with infinitely long, rodlike systems. The last part is devoted to the phenomenon of overcharging for colloidal particles and its explanation in terms of simple electrostatic arguments.

cond-mat.soft↗

arXiv2001

The Osmotic Coefficient of Rod-like Polyelectrolytes: Computer Simulation, Analytical Theory, and Experiment

The osmotic coefficient of solutions of rod-like polyelectrolytes is considered by comparing current theoretical treatments and simulations to recent experimental data. The discussion is restricted to the case of monovalent counterions and dilute, salt-free solutions. The classical Poisson-Boltzmann solution of the cell model correctly predicts a strong decrease in the osmotic coefficient, but upon closer look systematically overestimates its value. The contribution of ion-ion-correlations are quantitatively studied by MD simulations and the recently proposed DHHC theory. However, our comparison with experimental data obtained on synthetic, stiff-chain polyelectrolytes shows that correlation effects can only partly explain the discrepancy. A quantitative understanding thus requires theoretical efforts beyond the restricted primitive model of electrolytes.

cond-mat.soft↗

arXiv1999

Z_2-Regge versus Standard Regge Calculus in two dimensions

We consider two versions of quantum Regge calculus. The Standard Regge Calculus where the quadratic link lengths of the simplicial manifold vary continuously and the Z_2-Regge Model where they are restricted to two possible values. The goal is to determine whether the computationally more easily accessible Z_2 model still retains the universal characteristics of standard Regge theory in two dimensions. In order to compare observables such as average curvature or Liouville field susceptibility, we use in both models the same functional integration measure, which is chosen to render the Z_2-Regge Model particularly simple. Expectation values are computed numerically and agree qualitatively for positive bare couplings. The phase transition within the Z_2-Regge Model is analyzed by mean-field theory.

hep-lat↗

arXiv1998

Lattice Models of Quantum Gravity

Standard Regge Calculus provides an interesting method to explore quantum gravity in a non-perturbative fashion but turns out to be a CPU-time demanding enterprise. One therefore seeks for suitable approximations which retain most of its universal features. The $Z_2$-Regge model could be such a desired simplification. Here the quadratic edge lengths $q$ of the simplicial complexes are restricted to only two possible values $q=1+εσ$, with $σ=\pm 1$, in close analogy to the ancestor of all lattice theories, the Ising model. To test whether this simpler model still contains the essential qualities of the standard Regge Calculus, we study both models in two dimensions and determine several observables on the same lattice size. In order to compare expectation values, e.g. of the average curvature or the Liouville field susceptibility, we employ in both models the same functional integration measure. The phase structure is under current investigation using mean field theory and numerical simulation.

hep-lat↗

arXiv1994

The critical behaviour of Ising spins on 2D Regge lattices

We performed a high statistics simulation of Ising spins coupled to 2D quantum gravity on toroidal geometries. The tori were triangulated using the Regge calculus approach and contained up to $512^2$ vertices. We used a constant area ensemble with an added $R^2$ interaction term, employing the $dl/l$ measure. We find clear evidence that the critical exponents of the Ising phase transition are consistent with the static critical exponents and do not depend on the coupling strength of the $R^2$ interaction term. We definitively can exclude for this type of model a behaviour as predicted by Boulatov and Kazakov [Phys. Lett. {\bf B186}, 379 (1987)] for Ising spins coupled to dynamically triangulated surfaces.

hep-lat↗

arXiv1993

High-Temperature Series Analyses of the Classical Heisenberg and XY Model

Although there is now a good measure of agreement between Monte Carlo and high-temperature series expansion estimates for Ising ($n=1$) models, published results for the critical temperature from series expansions up to 12{\em th} order for the three-dimensional classical Heisenberg ($n=3$) and XY ($n=2$) model do not agree very well with recent high-precision Monte Carlo estimates. In order to clarify this discrepancy we have analyzed extended high-temperature series expansions of the susceptibility, the second correlation moment, and the second field derivative of the susceptibility, which have been derived a few years ago by Lüscher and Weisz for general $O(n)$ vector spin models on $D$-dimensional hypercubic lattices up to 14{\em th} order in $K \equiv J/k_B T$. By analyzing these series expansions in three dimensions with two different methods that allow for confluent correction terms, we obtain good agreement with the standard field theory exponent estimates and with the critical temperature estimates from the new high-precision MC simulations. Furthermore, for the Heisenberg model we reanalyze existing series for the susceptibility on the BCC lattice up to 11{\em th} order and on the FCC lattice up to 12{\em th} order.

hep-lat↗

arXiv1992

High precision single-cluster Monte Carlo measurement of the critical exponents of the classical 3D Heisenberg model

We report measurements of the critical exponents of the classical three-dimensional Heisenberg model on simple cubic lattices of size $L^3$ with $L$ = 12, 16, 20, 24, 32, 40, and 48. The data was obtained from a few long single-cluster Monte Carlo simulations near the phase transition. We compute high precision estimates of the critical coupling $K_c$, Binder's parameter $U^* and the critical exponents $ν,β/ ν, η$, and $α/ ν$, using extensively histogram reweighting and optimization techniques that allow us to keep control over the statistical errors. Measurements of the autocorrelation time show the expected reduction of critical slowing down at the phase transition as compared to local update algorithms. This allows simulations on significantly larger lattices than in previous studies and consequently a better control over systematic errors in finite-size scaling analyses.

hep-lat↗