Search results for "Hard spheres"
showing 10 items of 66 documents
A comparative study on the phase behaviour of highly charged colloidal spheres in a confining wedge geometry
2005
We studied the structures formed in aqueous dispersions of charged colloidal spheres under a constant low salt concentration of c = 6 × 10−6 mol l−1. Particles of diameter 2a = 1000 nm were confined to a low angle wedge geometry with plate separation 0<S<50 µm and observed with video microscopy. Irrespective of the initial particle density n we reproducibly observe the particles to migrate to the narrow wedge side on the timescale of a few days. Thereby an interface between a crystalline structure and a near particle free region is formed, which propagates slowly until the dilute region is exhausted of particles. While the origin of this separation is still unclear, the final extension of t…
Effects of confinement and external fields on structure and transport in colloidal dispersions in reduced dimensionality
2012
In this work, we focus on low-dimensional colloidal model systems, via simulation studies and also some complementary experiments, in order to elucidate the interplay between phase behavior, geometric structures and transport properties. In particular, we try to investigate the (nonlinear!) response of these very soft colloidal systems to various perturbations: uniform and uniaxial pressure, laser fields, shear due to moving boundaries and randomly quenched disorder.We study ordering phenomena on surfaces or in monolayers by Monte Carlo computer simulations of binary hard-disk mixtures, the influence of a substrate being modeled by an external potential. Weak external fields allow a control…
High-pressure phases, vibrational properties, and electronic structure ofNe(He)2andAr(He)2: A first-principles study
2009
We have carried out a comprehensive first-principles study of the energetic, structural, and electronic properties of solid rare-gas RG-helium binary compounds, in particular, NeHe2 and ArHe2, under pressure and at temperatures within the range of 0T2000 K. Our approach is based on density-functional theory and the generalized gradient approximation for the exchange-correlation energy; we rely on total Helmholtz freeenergy calculations performed within the quasiharmonic approximation for most of our analysis. In NeHe2, we find that at pressures of around 20 GPa the system stabilizes in the MgZn2 Laves structure, in accordance to what was suggested in previous experimental investigations. In…
Glass transition for dipolar hard spheres: A mode-coupling approach
1998
Abstract We apply the self-consistent mode-coupling equations, which were recently derived for molecular liquids, to a system of dipolar hard spheres. Making use of the direct correlation function in a mean spherical approximation and with a restriction of the rotational quantum number 1 to zero and one, we find three different phases in the η—T phase space. η and T denote the packing fraction and the temperature respectively. There is one phase where both the transitional degrees of freedom (TDOFs) and the orientational degrees of freedom (ODOFs) are ergodic (liquid), another phase with frozen TDOFs and ergodic ODOFs, and a third phase where TDOFs and ODOFs are frozen (glass). The dynamica…
Brownian dynamics simulations of colloidal hard spheres. Effects of sample dimensionality on self-diffusion
1994
The self-diffusion coefficients of colloidal hard spheres were determined by Brownian dynamics (BD) computer simulations using a new efficient algorithm for treatment of the hard-sphere interactions. Calculations were done on an Apple PC type MacIIcx and on a Micro VAX 3000, considering samples in two and three dimensions at varying particle concentrations. Our results in three dimensions are compared with experimental results from our own group which were obtained by forced Rayleigh scattering (FRS), and with numerical results from a dynamical Monte Carlo simulation by Cichocki and Hinsen. Good agreement with the latter was found for particle volume fractions up to 0.40. Differences in the…
Microscopic dynamics of molecular liquids and glasses: Role of orientations and translation-rotation coupling
2001
We investigate the dynamics of a fluid of dipolar hard spheres in its liquid and glassy phase, with emphasis on the microscopic time or frequency regime. This system shows rather different glass transition scenarios related to its rich equilibrium behavior which ranges from a simple hard sphere fluid to a long range ferroelectric orientational order. In the liquid phase close to the ideal glass transition line and in the glassy regime a medium range orientational order occurs leading to a softening of an orientational mode. To investigate the role of this mode we use the molecular mode-coupling equations to calculate the spectra $\phi_{lm}^{\prime \prime}(q,\omega)$ and $\chi _{lm}''(q,\ome…
A generalization of the Carnahan–Starling approach with applications to four- and five-dimensional hard spheres
2018
Abstract Development of good equations of state for hard spheres is an important task in the study of real fluids. In a way consistent with other theoretical results, we generalize the famous Carnahan–Starling approach for arbitrary dimensions and apply it to four- and five-dimensional hard spheres. We obtain simple and integer representations for virial coefficients of lower orders and accurate equations of state. Since theoretically and practically validated, these results improve understanding of hard sphere fluids.
Fluids in extreme confinement.
2012
For extremely confined fluids with two-dimensional density $n$ in slit geometry of accessible width $L$, we prove that in the limit $L\to 0$ the lateral and transversal degrees of freedom decouple, and the latter become ideal-gas-like. For small wall separation the transverse degrees of freedom can be integrated out and renormalize the interaction potential. We identify $n L^2 $ as hidden smallness parameter of the confinement problem and evaluate the effective two-body potential analytically, which allows calculating the leading correction to the free energy exactly. Explicitly, we map a fluid of hard spheres in extreme confinement onto a 2d-fluid of disks with an effective hard-core diame…
Experimental Evidence for a Structural-Dynamical Transition in Trajectory Space.
2016
Among the key insights into the glass transition has been the identification of a non-equilibrium phase transition in trajectory space which reveals phase coexistence between the normal supercooled liquid (active phase) and a glassy state (inactive phase). Here we present evidence that such a transition occurs in experiment. In colloidal hard spheres we find a non-Gaussian distribution of trajectories leaning towards those rich in locally favoured structures (LFS), associated with the emergence of slow dynamics. This we interpret as evidence for an non-equilibrium transition to an inactive LFS-rich phase. Reweighting trajectories reveals a first-order phase transition in trajectory space be…
Anisotropic pair correlations in binary and multicomponent hard-sphere mixtures in the vicinity of a hard wall: A combined density functional theory …
2015
The fundamental measure approach to classical density functional theory has been shown to be a powerful tool to predict various thermodynamic properties of hard-sphere systems. We employ this approach to determine not only one-particle densities but also two-particle correlations in binary and six-component mixtures of hard spheres in the vicinity of a hard wall. The broken isotropy enables us to carefully test a large variety of theoretically predicted two-particle features by quantitatively comparing them to the results of Brownian dynamics simulations. Specifically, we determine and compare the one-particle density, the total correlation functions, their contact values, and the force dis…