Comparison of two representations of a random cut of identical sphere packing

We compare two-dimensional froths obtained by radical tessellation of random planar cuts made through disordered assemblies of monosize spheres at different packing fractions C from C=0 to C=0.64 with two-dimensional stereological cuts obtained through the three-dimensional froths made with the same packing. We have built numerically the packings using different algorithms. The study of both topological and metric properties shows significant differences between the two representations. Received 26 May 1999 and Received in final form 13 November 1999     

Structural properties of amorphous TiO<Subscript>2</Subscript> nanoparticles

Structural properties of amorphous TiO₂ spherical nanoparticles have been studied in models with different sizes of 2 nm, 3 nm, 4 nm and 5 nm under non-periodic boundary conditions. We use the pairwise interatomic potentials proposed by Matsui and Akaogi. Models have been obtained by cooling from the melt via molecular dynamics (MD) simulation. Structural properties of an amorphous nanoparticle obtained at 350 K have been analyzed in detail through the partial radial distribution functions (PRDFs), coordination number distributions, bond-angle distributions and interatomic distances. Moreover, we show the radial density profile in a nanoparticle. Calculations show that size effects on structure of a model are significant and that if the size is larger than 3 nm, amorphous TiO₂ nanoparticles have a distorted octahedral network structure with the mean coordination number Z_Ti-O ≈6.0 and Z_O-Ti ≈3.0 like those observed in the bulk. Surface structure and surface energy of nanoparticles have been obtained and presented.     

Vertically shaken column of spheres. Onset of fluidization

The onset of surface fluidization of granular material in a vertically vibrated container, z = A cosωt , is studied experimentally. Recently, for a column of spheres it has been theoretically found (see T. P?schel, T. Schwager, C. Salue na, Phys. Rev. E 62, 1361 (2000)) that the particles lose contact if a certain condition for the acceleration amplitude ≡Aω²/g = f (ω) holds. This result is in disagreement with other findings where the criterion = = const was found to be the criterion of fluidization. We show that for a column of spheres a critical acceleration is not a proper criterion for fluidization and compare the results with theory. Received 21 August 2000 and Received in final form 30 October 2000     

Statistical verification of crystallization in hard sphere packings under densification

The performance of various structure characteristics in the task of indicating structural peculiarities in packings of hard spheres is investigated. Various characteristics based on Voronoi polyhedra, spherical harmonics, and Delaunay simplices are considered together with the pair correlation function and the mean number of r-close triples. They are applied to a set of hard sphere packings of density φ from 0.62 to 0.72. It turns out that all used structure characteristics are able to indicate changes of order from non-crystalline to crystalline packings. However, not all of them are sensitive enough to indicate different stages of structure transformation under densification. The characteristics based on Delaunay simplices turn out to be the most sensitive for this purpose. For the models considered three principal structure classes are found: packings of densities lower than the known critical value 0.64 showing a non-crystalline behavior; packings with considerable crystalline regions for φ up to 0.66–0.67; rather complete crystals although with numerous defects for φ above 0.67.     

Field-induced realignment of a smectic nanodroplet in an external magnetic field: A numerical investigation

The field-induced realignment of a smectic-A phase is in principle a complicated process involving the director rotation via the interaction with the field and the layer rotation via the molecular interactions. Time-resolved X-ray scattering experiments have revealed major phenomena concerning the maintenance of the integrity of the smectic-A layer structure during the alignment process. In order to obtain a deeper insight into this process, we have carried out a dissipative particle dynamics study of the realignment kinetics of a nanodroplet of a smectic-A liquid crystal suspended in an isotropic fluid following a switch in the direction of an applied magnetic field. The strength of the mesogen-field interaction is small compared to the inter-molecular interactions. The reaction of the smectic configuration to the field switch was found to depend on the balance between the inter-molecular interactions stabilising the formation of the smectic layering and the interaction of the mesogens with the external field. It is found that the rotational behaviour of the smectic layers under the influence of an external magnetic field arises from a combination of stochastic translational displacements and rotational motions of the centres of mass of the mesogens in the nanodroplets. The simulations indicate that X-ray scattering and NMR experiments monitoring the orientational order are sensitive to different aspects of the realignment process.     

A dissipative particle dynamics study of the realignment of a nanodroplet of a nematic in a weak external magnetic field

We present a dissipative particle dynamics (DPD) approach for simulating the realignment of a nematic nanodroplet suspended in an isotropic fluid following a switch in the direction of an applied external magnetic field. The interaction of the mesogens with the external field is weak relative to the inter-molecular interactions. The simulations were used to investigate the way orientational equilibrium is re-established. The results reveal that the realignment process of the nanodroplet is consistent with its fluid structure. The reorientation of the nanodroplet as a whole is found to be caused by an internal structural rearrangement rather than a coherent rotation of the centres of mass of the mesogens about the centre of the nanodroplet. The switch in the field direction furthermore is found to induce a transient spatial variation in the orientational order of the long axes of the mesogens: the orientational order parameters decreases on moving from the core of the nanodroplet to the surface in contact with the isotropic environment. The results highlight differences between the time evolution of the orientation of the long molecular axes in the field and the rotations of the centres of mass of the mesogens about the centre of the nanodroplet.     

Can a difference in molecular weights cause an eruption in a driven flow of self-organizing immiscible system?

Driven flow of a non-equilibrium non-conservative (NENC) system with a mixture of immiscible particles (A,B of molecular weight M_A, M_B) exhibits self-organizing patterns (segregation, phase-separation, etc.) in steady-state. The flow response (v) of mass flux density (j) to bias (H), in steady-state is found to be sensitive to molecular weight ratio (α = M_B/M_A). While the flux density (j) responds linearly to bias for both components (A, B) at α = 1, onset of eruptive response occurs at extreme bias (H ↦ 1) at α > 1 where v ↦∞ for heavier (B) and v ↦- ∞ for lighter (A) constituents. Difference in molecular weights (M_A, M_B) is not only critical to eruptive flow but also in controlling the flow response prior to this crossover.     

Restructuring of force networks

The compaction of granular packings or soils is a collective process which for higher densities becomes increasingly slower reaching glassy behaviour. We present a study of this problem from various points of view, in particular we will represent the evolving force network that percolates through the system by an inverse fiber rupture model. Received 15 March 2002 and Received in final form 29 July 2002     

Pore size distribution in porous glass: fractal dimension obtained by calorimetry

By differential Scanning Calorimetry (DSC), at low heating rate and using a technique of fractionation, we have measured the equilibrium DSC signal (heat flow) J _q ⁰ of two families of porous glass saturated with water. The shape of the DSC peak obtained by these techniques is dependent on the sizes distribution of the pores. For porous glass with large pore size distribution, obtained by sol-gel technology, we show that in the domain of ice melting, the heat flow J_q is related to the melting temperature depression of the solvent, ΔT _m , by the scaling law: J _q ⁰∼ΔT _m ^{- (1 + D)}. We suggest that the exponent D is of the order of the fractal dimension of the backbone of the pore network and we discuss the influence of the variation of the melting enthalpy with the temperature on the value of this exponent. Similar D values were obtained from small angle neutron scattering and electronic energy transfer measurements on similar porous glass. The proposed scaling law is explained if one assumes that the pore size distribution is self similar. In porous glass obtained from mesomorphic copolymers, the pore size distribution is very sharp and therefore this law is not observed. One concludes that DSC, at low heating rate ( q? 2^°C/min) is the most rapid and less expensive method for determining the pore distribution and the fractal exponent of a porous material. Received 23 July 1999 and Received in final form 16 February 2001     

Dynamical properties of Ag-Cu binary alloy from molecular dynamics simulation

Molecular dynamics simulations (MD) of dynamical properties of molten binary Ag-Cu alloy is presented at various temperature above the eutetic temperature. Atoms in the system have been modelled through an interatomic Lennard-Jones potential interaction. The structure, through the effective pair distribution function allows to determine the Enksog collision frequency as well as the coordination of atoms in the first shell. The surface traction, which is the force per unit area between the species shows a long separation oscillation about the value zero, while the collision frequency of pairs of atoms increase with increasing temperature. The adhesion energy between components found to be 3.4178 J/m². In agreement with theory, we found a decrease in surface tension of Ag-Cu alloy as temperature increases. Separation of atoms pairs in the first shell might be responsible for a non linear relationship found between temperature and coordination number in present calculations.     

Interatomic potential effects on dynamical heterogeneities in liquid SiO2

Dynamical heterogeneities (DH) in low density liquid SiO₂ have been investigated by molecular dynamics (MD) method. Simulations were done in the basic cube under periodic boundary conditions containing 3000 particles with the pair interatomic potentials, which have a weak electrostatic interaction and a Morse type short range interaction (PMSI). We have evaluated the non-Gaussian parameter for the self part of the van Hove correlation function and we found a clear evidence of the existence of DH in low density liquid SiO₂. Moreover, the atomic displacement distribution (ADD) in a model has been obtained and it deviates from a Gaussian form. The results have been compared with those obtained in another liquid SiO₂ system with the Born-Mayer interatomic potentials (BMP) in order to observe the interatomic potential effects on the DH in the system and indeed, the effects are strong. Calculations showed that particles of extremely low or fast mobility have a tendency to form a cluster and mean cluster size of most mobile and immobile particles in PMSI models increases with decreasing temperature. In contrast, no systematic changes have been obtained for the most mobile and immobile particles in BMP models. Calculations show that there is no relation between local particle environment and particle mobility in the system.     

Structure and properties of confined sodium nitrite

We study the lateral and transverse diffusion of amphiphiles in two-component bilayer membranes, using a coarse-grained model for amphiphilic molecules and combined Monte Carlo-Molecular Dynamics simulations. Membrane structural properties, such as the mean thickness, are also measured. The dependence of such properties on membrane composition, inter-molecular interactions, and amphiphile stiffness is determined. In particular, we show that addition of shorter amphiphiles drives the model membrane towards a more fluid state, with increased amphiphile lateral diffusion rates. These results can be understood in the framework of a simple free-volume model. Furthermore, we observe an increase in the trans-membrane diffusion when the interaction energy of amphiphiles with their neighboring molecules is decreased. Received: 6 December 2002 / Accepted: 17 April 2003 / Published online: 27 May 2003 RID="a" ID="a"e-mail: imparato@mpikg-golm.mpg.de RID="b" ID="b"e-mail: shillcock@mpikg-golm.mpg.de RID="c" ID="c"e-mail: lipowsky@mpikg-golm.mpg.de     

Aging and energy landscapes: application to liquids and glasses

The equation of state for a liquid in equilibrium, written in the potential energy landscape formalism, is generalized to describe out-of-equilibrium conditions. The hypothesis that during aging the system explores basins associated to equilibrium configurations is the key ingredient in the derivation. Theoretical predictions are successfully compared with data from molecular dynamics simulations of different aging processes, such as temperature and pressure jumps. Received 7 August 2002 / Received in final form 8 October 2002 Published online 19 December 2002 RID="a" ID="a"Present address: Laboratoire de Physique Théorique des Liquides, Université Pierre et Marie Curie, 4 place Jussieu, Paris 75005, France e-mail: mossa@lptl.jussieu.fr     

Model of silica glass from combined classical and ab initio molecular-dynamics simulations

A Car-Parrinello (CP) molecular dynamics simulation of vitreous silica, combined with classical molecular dynamics, is presented. The equilibration of the liquid, quench and relaxation of the glass are performed classically using the van Beest, Kramer and van Santen (BKS) potential [12] and the resulting configuration (coordinates and velocities) is used as input for the CP simulation. A remarkable stability of the CP dynamics is observed justifying this procedure and validating the BKS potential. Several structural and electronic properties are calculated and compared with experiments. Received 23 March 1999 and Received in final form 15 July 1999     

Probability distribution of inherent states in models of granular media and glasses

The present paper develops a Statistical Mechanics approach to the inherent states of glassy systems and granular materials by following the original ideas proposed by Edwards for granular media. We consider three lattice models (a diluted spin glass, a system of hard spheres under gravity and a hard-spheres binary mixture under gravity) introduced to describe glassy and granular systems. They are evolved using a “tap dynamics” analogous to that of experiments on granular media. We show that the asymptotic states reached in such a dynamics are not dependent on the particular sample history and are characterized by a few thermodynamical parameters. We assume that under stationarity these systems are distributed in their inherent states satisfying the principle of maximum entropy. This leads to a generalized Gibbs distribution characterized by new “thermodynamical” parameters, called “configurational temperatures” (related to Edwards compactivity for granular materials). Finally, we show by Monte Carlo calculations that the average of macroscopic quantities over the tap dynamics and over such distribution indeed coincide. In particular, in the diluted spin glass and in the system of hard spheres under gravity, the asymptotic states reached by the system are found to be described by a single “configurational temperature”. Whereas in the hard-spheres binary mixture under gravity the asymptotic states reached by the system are found to be described by two thermodynamic parameters, coinciding with the two configurational temperatures which characterize the distribution among the inherent states when the principle of maximum entropy is satisfied under the constraint that the energies of the two species are independently fixed. Received 19 March 2002 and Received in final form 14 June 2002     

Helical close packings of ideal ropes

An adsorption-desorption (or parking-lot) model can reproduce qualitatively the densification kinetics and other features of a weakly vibrated granular material. Here we study the the two-time correlation and response functions of the model and demonstrate that their behavior is consistent with recently observed memory effects in granular materials. Although the densification kinetics and hysteresis are robust properties, we show that the aging behavior of the adsorption-desorption model is different from other models of granular compaction. We propose an experimental test to distinguish the possible aging behaviors. Received 26 February 2001     

Dewetting on porous media with aspiration

We consider a porous solid covered with a water film (or with a drop) in situations where the liquid is pumped in, either spontaneously (if the porous medium is hydrophilic) or mechanically (by an external pump). The dynamics of dewetting is then strongly modified. We analyse a few major examples, a) horizontal films, which break at a certain critical thickness, b) the “modified Landau-Levich problem” where a porous plate moves up from a bath and carries a film: aspiration towards the plate limits the height H reached by the film, c) certain situation where the hysteresis of contact angles is important. Received 5 October 1999 and Received in final form 7 February 2000     

Living polymers in random media: a 2D Monte-Carlo investigation on a square lattice

The evolution of the mean chain length and mean end to end square radius of a two dimensional system of living polymers at constant monomer concentration is studied as a function of the obstacle density . The fact that the system adapts the mean chain length in order to reduce the entropic constraint does not lead to a different asymptotic dependence of on than what is observed for dead polymers. The change of the molecular weight distribution form in the presence of obstacles suggests that a Levy flight could appear in system of wormlike micelles in a porous medium. Received: 1 September 1997 / Received in final form: 22 January 1998 / Accepted: 30 January 1998     

Echo tracer dispersion in flows of polymer solutions through porous media: A tool for detecting weak permeability heterogeneities?

Tracer dispersion in Newtonian and shear-thinning fluids (scleroglucan-water polymer solutions) flowing through single and double porosity grain packings has been studied experimentally using both classical transmission dispersion and echo dispersion (in the latter, the concentration variation front is pumped back through a detector at the inlet after penetrating for a chosen distance into the sample). Transmission dispersion increases markedly in both types of samples with the shear thinning index of the fluid at all Péclet numbers (except when molecular diffusion is dominant). Echo and transmission experiments give nearly identical dispersivity values for Newtonian fluids while echo dispersivity is lower than transmission for shear thinning ones. The normalized dispersivity difference has same order of magnitude for single and double porosity samples and increases with the shear thinning exponent α (by a factor of 2 between α = 0.35 and α = 0.60). This difference may be due to heterogeneities inducing permeability variations of small amplitude over distances of the order of the sample section : their influence on tracer dispersion is partly reversible with respect to a change of the flow direction and is only detectable if it is amplified by the shear-thinning properties of the fluid. Received 19 September 2001