0000000000012990
AUTHOR
K. Binder
Polymer brushes in solvents of variable quality: Molecular dynamics simulations using explicit solvent
The structure and thermodynamic properties of a system of end-grafted flexible polymer chains grafted to a flat substrate and exposed to a solvent of variable quality are studied by molecular dynamics methods. The macromolecules are described by a coarse-grained bead-spring model, and the solvent molecules by pointlike particles, assuming Lennard-Jones-type interactions between pairs of monomers (epsilon(pp)), solvent molecules (epsilon(ss)), and solvent monomer (epsilon(ps)), respectively. Varying the grafting density sigma(g) and some of these energy parameters, we obtain density profiles of solvent particles and monomers, study structural properties of the chain (gyration radius componen…
Monte Carlo Simulation of Polymeric Materials — Still a Challenge?
Monte Carlo simulation of polymeric materials is difficult, since they exhibit nontrivial structure over many different length scales, from the bond length (∼1A) to the radius of the random coil (∼102A) and still larger collective length scales, and similarly, motions occur on very different time scales. Hence it is a nontrivial problem to devise suitable coarse-grained models which capture the essential physics and are accessible to simulation.
Classical Statistical Mechanics
Some aspects of statistical mechanics that are particularly important for computer simulation approaches are recalled. Using Ising and classical Heisenberg models as examples, various statistical ensembles and appropriate thermodynamic potentials are introduced, and concepts such as Legendre transformations between ensembles and the thermodynamic integration method to obtain the entropy are mentioned. Probability distributions characterizing statistical fluctuations are discussed, fluctuation relations for response functions are derived, and the behavior of these quantities at first and second order phase transitions are described qualitatively. Also the general consequences of phase coexis…
I. Glass Transition. Theoretical concepts on the glass transition of polymers and their test by computer simulation
Various organic molecules, in particular polymers, are extremely good glass formers and allow the study of supercooled melts near the glass transition in metastable equilibrium. Theories of the glass transition imply such an equilibrium (e.g. mode-coupling theory, or Gibbs-di Marzio theory) and can hence be tested in these systems. Simplified lattice models for polymer melts (e.g. the bond fluctuation model) have been developed that can very efficiently be studied by Monte-Carlo simulation, and although they fail to accurately describe the local structure, they describe many features of the experiments very well. In this model, the mechanism of the glass transition is a competition between …
Simulation of Models for Isotropic and Anisotropic Orientational Glasses
“Orientational glass” behavior is found when molecular crystals are randomly diluted, and quadrupole moments get frozen by random alignment of the molecules, similar to “spin glass” behavior of randomly diluted magnets. Monte Carlo simulation of lattice models where quadrupole moments interact with nearest neighbor Gaussian coupling is a unique tool to study this behavior. The time-dependent glass order parameter exhibits anomalously slow relaxation, compatible with the Kohlrausch-Williams-Watts (KWW) stretched exponential function. Both isotropic and anisotropic models exhibit in d=2 and d=3 spatial dimensions glass transitions at zero temperature only. While the glass correlation length a…
Two-dimensional model colloids and nano wires: phase transitions, effects of external potentials and quantum effects
Abstract Quantum effects, structures and phase transitions in Nano-systems have been analyzed. An overview is given on the results of our computations on structural and elastic properties of model colloids, on phase transitions of model colloids in external fields, and on structural and electronic properties of stretched atomic wires.
The Mixed Akali Effect in Ternary Alkali Silicate Melts: Insight from Molecular Dynamics Computer simulations
Large scale molecular dynamics (MD) computer simulations are used to study the amorphous alkali silicates (Li2O)(2·SiO2) [LS2], (K2O)(2·SiO2) [KS2], and (0.5·Li2O)(0.5·K2O)(2·SiO2) [LKS2]. These systems are characterized by a fast alkali ion motion in a relatively immobile Si-0 matrix. We investigate the so-called mixed alkali effect (MAE) which is reflected as a significant decrease of the alkali ion diffusion constants in LKS2 as compared to the corresponding binary systems LS2 and KS2. We show that the subtle interplay between the structure on intermediate length scales and the alkali diffusion is important to understand the microscopic origin of the MAE.