Fragility in p-spin models

We investigate the relation between fragility and phase space properties - such as the distribution of states - in the mean field p-spin model, a solvable model that has been frequently used in studies of the glass transition. By direct computation of all the relevant quantities, we find that: i) the recently observed correlation between fragility and vibrational properties at low temperature is present in this model; ii) the total number of states is a decreasing function of fragility, at variance of what is currently believed. We explain these findings by taking into account the contribution to fragility coming from the transition paths between different states. Finally, we propose a geometric picture of the phase space that explains the correlation between properties of the transition paths, distribution of states and their vibrational properties. However, our analysis may not apply to strong systems where inflection points in the configurational entropy as a function of the temperature are found

Potential energy topology and relaxation processes in a model glass

We use computer simulation to investigate the topology of the potential energy $V(\{{\bf R}\})$ and to search for doublewell potential's (DWP) in a model glass . By a sequence of Newtonian and dissipative dynamics we find different minima of $V(\{{\bf R}\})$ and the energy profile along the least action paths joining them. At variance with previous suggestions, we find that the parameters describing the DWP's are correlated among each others. Moreover, the trajectory of the system in the 3$N$-d configurational phase space follows a quasi-1-d manifold. The motion parallel to the path is characterized by jumps between minima, and is nearly uncorrelated from the orthogonal, harmonic, dynamics.Comment: 4 pages, RevTex, 4 PostScript figure

More on phase diagram of Laponite

The phase diagram of a charged colloidal system (Laponite) has been investigated by dynamic light scattering in a previously unexplored range of salt and clay concentrations. Specifically the clay weight and salt molar concentrations have been varied in the ranges Cw=0.004- 0.025, Cs=(1x 10^-3- 5x 10^-3) M respectively. As in the case of free salt water samples (Cs= 1x 10^-4 M) an aging dynamics towards two different arrested phases is found in the whole examined Cw and Cs range. Moreover a transition between these two different regimes is found for each investigated salt concentration. It is clear from these measurements that a revision of the phase diagram is necessary and a new "transition" line between two different arrested states is drawn.Comment: 16 pages, 5 figures, submitted to Langmui

Routes to gelation in a clay suspension

The gelation of water suspension of a synthetic clay (Laponite) has been studied by dynamic light scattering in a wide range of clay weight concentration (Cw = 0.003-0.031). At variance with previous determination, indicating a stable liquid phase for Cw < Cw*=0.015-0.018, we find that the gelation takes actually place in the whole examined Cw range. More importantly, we find that Cw* marks the transition between two different routes to gelation. We hypothesize that at low concentration Laponite suspension behaves as an attractive colloid and that the slowing down of the dynamics is attained by the formation of larger and larger clusters while at high concentration the basic units of the gel could be the Debye Huckel spheres associated to single Laponite plates.Comment: 5 pages, 4 figure

Acoustic attenuation in glasses and its relation with the boson peak

A theory for the vibrational dynamics in disordered solids [W. Schirmacher, Europhys. Lett. {\bf 73}, 892 (2006)], based on the random spatial variation of the shear modulus, has been applied to determine the wavevector ($k$) dependence of the Brillouin peak position ($\Omega_k)$ and width ($\Gamma_k$), as well as the density of vibrational states ($g(\omega)$), in disordered systems. As a result, we give a firm theoretical ground to the ubiquitous $k^2$ dependence of $\Gamma_k$ observed in glasses. Moreover, we derive a quantitative relation between the excess of the density of states (the boson peak) and $\Gamma_k$, two quantities that were not considered related before. The successful comparison of this relation with the outcome of experiments and numerical simulations gives further support to the theory.Comment: To appear on PR

Influence of an adsorbing polymer in the aging dynamics of Laponite clay suspensions

Clay-polymer dispersions in aqueous solutions have attracted a great interest in recent years due to their industrial applications and intriguing physical properties. Aqueous solutions of bare Laponite particles are known to age spontaneously from an ergodic state to a non ergodic state in a time varying from hours to months depending on Laponite concentration. When a polymer species like Polyethylene Oxide (PEO) is added to the solution, it weakly adsorbs on clay particle surfaces modifying the effective interaction potential between Laponite particles. A dynamic light scattering study, varying polymer concentration at fixed polymer molecular weight (Mw=200.000 g/mol), has been performed in order to understand the effect of polymer on the aging dynamics of the system. The results obtained show that arresting phenomena between clay particles are hindered if PEO is added and consequently the aging dynamics slows down with increasing PEO concentration. This process is possibly due to the progressive coverage of the clay surface by polymers that grow with increasing PEO concentration and may lead to steric stabilization.Comment: 13 pages, 6 figures, manuscript accepted for publication on Philosophical Magazin

Orientational and induced contributions to the depolarized Rayleigh spectra of liquid and supercooled ortho-terphenyl

The depolarized light scattering spectra of the glass forming liquid ortho-terphenyl have been calculated in the low frequency region using molecular dynamics simulation. Realistic system's configurations are produced by using a recent flexible molecular model and combined with two limiting polarizability schemes, both of them using the dipole-induced-dipole contributions at first and second order. The calculated Raman spectral shape are in good agreement with the experimental results in a large temperature range. The analysis of the different contributions to the Raman spectra emphasizes that the orientational and the collision-induced (translational) terms lie on the same time-scale and are of comparable intensity. Moreover, the cross terms are always found to be an important contribution to the scattering intensity.Comment: RevTeX4, 7 pages, 8 eps figure

Heat capacity of liquids: A hydrodynamic approach

We study autocorrelation functions of energy, heat and entropy densities obtained by molecular dynamics simulations of supercritical Ar and compare them with the predictions of the hydrodynamic theory. It is shown that the predicted by the hydrodynamic theory single-exponential shape of the entropy density autocorrelation functions is perfectly reproduced for small wave numbers by the molecular dynamics simulations and permits the calculation of the wavenumber-dependent specific heat at constant pressure. The estimated wavenumber-dependent specific heats at constant volume and pressure, $C_{v}(k)$ and $C_{p}(k)$, are shown to be in the long-wavelength limit in good agreement with the macroscopic experimental values of $C_{v}$ and $C_{p}$ for the studied thermodynamic points of supercritical Ar.Comment: 8 pages, 5 figure

Fluctuations of entropy production in the isokinetic ensemble

We discuss the microscopic definition of entropy production rate in a model of a dissipative system: a sheared fluid in which the kinetic energy is kept constant via a Gaussian thermostat. The total phase space contraction rate is the sum of two statistically independent contributions: the first one is due to the work of the conservative forces, is independent of the driving force and does not vanish at zero drive, making the system non-conservative also in equilibrium. The second is due to the work of the dissipative forces, and is responsible for the average entropy production; the distribution of its fluctuations is found to verify the Fluctuation Relation of Gallavotti and Cohen. The distribution of the fluctuations of the total phase space contraction rate also verify the Fluctuation Relation. It is compared with the same quantity calculated in the isoenergetic ensemble: we find that the two ensembles are equivalent, as conjectured by Gallavotti. Finally, we discuss the implication of our results for experiments trying to verify the validity of the FR.Comment: 8 pages, 4 figure