arXiv subjects

R. Di Leonardo

Publications and source records attributed to R. Di Leonardo.

35 records · Page 2Linked to original sources

arXiv2006

Aging after shear rejuvenation in a soft glassy colloidal suspension: evidence for two different regimes

The aging dynamics after shear rejuvenation in a glassy, charged clay suspension have been investigated through dynamic light scattering (DLS). Two different aging regimes are observed: one is attained if the sample is rejuvenated before its gelation and one after the rejuvenation of the gelled sample. In the first regime, the application of shear fully rejuvenates the sample, as the system dynamics soon after shear cessation follow the same aging evolution characteristic of normal aging. In the second regime, aging proceeds very fast after shear rejuvenation, and classical DLS cannot be used. An original protocol to measure an ensemble averaged intensity correlation function is proposed and its consistency with classical DLS is verified. The fast aging dynamics of rejuvenated gelled samples exhibit a power law dependence of the slow relaxation time on the waiting time.

cond-mat.soft↗

arXiv2005

Hard sphere-like dynamics in a non hard sphere liquid

The collective dynamics of liquid Gallium close to the melting point has been studied using Inelastic X-ray Scattering to probe lengthscales smaller than the size of the first coordination shell. %(momentum transfers, $Q$, $>$15 nm$^{-1}$). Although the structural properties of this partially covalent liquid strongly deviate from a simple hard-sphere model, the dynamics, as reflected in the quasi-elastic scattering, are beautifully described within the framework of the extended heat mode approximation of Enskog's kinetic theory, analytically derived for a hard spheres system. The present work demonstrates the applicability of Enskog's theory to non hard- sphere and non simple liquids.

cond-mat.dis-nn↗

arXiv2004

Aging under Shear: Structural Relaxation of a Non-Newtonian Fluid

The influence of an applied shear field on the dynamics of an aging colloidal suspension has been investigated by the dynamic light scattering determination of the density autocorrelation function. Though a stationary state is never observed, the slow dynamics crosses between two different non-equilibrium regimes as soon as the structural relaxation time approaches the inverse shear rate. In the shear dominated regime (at high shear rate values) the structural relaxation time is found to be strongly sensitive to shear rate while aging proceeds at a very slow rate. The effect of shear on the detailed shape of the density autocorrelation function is quantitatively described assuming that the structural relaxation process arises from the heterogeneous superposition of many relaxing units each one independently coupled to shear with a parallel composition rule for timescales.

cond-mat.soft↗

arXiv2003

High frequency dynamics in a monatomic glass

The high frequency dynamics of glassy Selenium has been studied by Inelastic X-ray Scattering at beamline BL35XU (SPring-8). The high quality of the data allows one to pinpoint the existence of a dispersing acoustic mode for wavevectors ($Q$) of $1.5<Q<12.5$ nm$^{-1}$, helping to clarify a previous contradiction between experimental and numerical results. The sound velocity shows a positive dispersion, exceeding the hydrodynamic value by $\approx$ 10% at $Q<3.5$ nm$^{-1}$. The $Q^2$ dependence of the sound attenuation $Γ(Q)$, reported for other glasses, is found to be the low-$Q$ limit of a more general $Γ(Q) \propto Ω(Q)^2$ law which applies also to the higher $Q$ region, where $Ω(Q)\propto Q$ no longer holds.

cond-mat.dis-nn↗

arXiv2003

A spectroscopic cell for fast pressure jumps across the glass transition line

We present a new experimental protocol for the spectroscopic study of the dynamics of glasses in the aging regime induced by sudden pressure jumps (crunches) across the glass transition line. The sample, initially in the liquid state, is suddenly brought in the glassy state, and therefore out of equilibrium, in a four-window optical crunch cell which is able to perform pressure jumps of 3 kbar in a time interval of ~10 ms. The main advantages of this setup with respect to previous pressure-jump systems is that the pressure jump is induced through a pressure transmitting fluid mechanically coupled to the sample stage through a deformable membrane, thus avoiding any flow of the sample itself in the pressure network and allowing to deal with highly viscous materials. The dynamics of the sample during the aging regime is investigated by Brillouin Light Scattering (BLS). For this purpose the crunch cell is used in conjunction with a high resolution double monochromator equipped with a CCD detector. This system is able to record a full spectrum of a typical glass forming material in a single 1 s shot. As an example we present the study of the evolution toward equilibrium of the infinite frequency longitudinal elastic modulus (M_infinity) of a low molecular weight polymer (Poly(bisphenol A-co-epichlorohydrin), glycidyl end capped). The observed time evolution of M_infinity, well represented by a single stretched exponential, is interpreted within the framework of the Tool-Narayanaswamy theory.

cond-mat.dis-nn↗

arXiv2002

Non-Equilibrium Thermodynamic Description of the Coupling between Structural and Entropic Modes in Supercooled Liquids

The density response of supercooled glycerol to an impulsive stimulated thermal grating (q=0.63 micron^-1) has been studied in the temperature range (T=200-340 K) where the structure rearrangement (alpha-relaxation) and thermal diffusion occur on the same time scale. A strong interaction between the two modes occurs giving rise to a dip in the T-dependence of the apparent thermal conductivity and a flattening of the apparent alpha-relaxation time upon cooling. A non-equilibrium thermodynamic (NET) model for the long time response of relaxing fluids has been developed. The model is capable to reproduce the experimental data and to explain the observed phenomenology.

cond-mat.dis-nn↗

arXiv2002

Experimental evidence for high frequency transverse-like excitations in glasses

The dynamic structure factor of glassy and liquid glycerol has been measured by inelastic X-ray scattering in the exchanged momentum ($Q$) region $Q$=2$÷$23 nm$^{-1}$ and in the temperature range 80$÷$570 K. Beside the propagating longitudinal excitations modes, at low temperature the spectra show a second non $Q$-dispersing peak at $\hbar Ω_T$$\approx$8.5 meV. We assign this peak to the transverse dynamics that, in topologically disordered systems, acquires a longitudinal symmetry component. This assignment is substantiated by the observation that, in the liquid, this peak vanishes when the structural relaxation time $τ_α$ approaches $Ω_T^{-1}$, a behavior consistent with the condition $τ_αΩ_T^{-1}$$>>$1 required for the existence of a transverse-like dynamics in the liquid state.

cond-mat.dis-nn↗

arXiv2002

Quasi-saddles as relevant points of the potential energy surface in the dynamics of supercooled liquids

The supercooled dynamics of a Lennard-Jones model liquid is numerically investigated studying relevant points of the potential energy surface, i.e. the minima of the square gradient of total potential energy $V$. The main findings are: ({\it i}) the number of negative curvatures $n$ of these sampled points appears to extrapolate to zero at the mode coupling critical temperature $T_c$; ({\it ii}) the temperature behavior of $n(T)$ has a close relationship with the temperature behavior of the diffusivity; ({\it iii}) the potential energy landscape shows an high regularity in the distances among the relevant points and in their energy location. Finally we discuss a model of the landscape, previously introduced by Madan and Keyes [J. Chem. Phys. {\bf 98}, 3342 (1993)], able to reproduce the previous findings.

cond-mat.soft↗

arXiv2001

Off-equilibrium dynamics in the energy landscape of a simple model glass

The aging dynamics of a simple model glass is numerically investigated observing how it takes place in the potential energy landscape $V$. Partitioning the landscape in basins of minima of $|\nabla V|^2$, we are able to elucidate some interesting topological properties of the aging process. The main result is the characterization of the long time behavior as a jump dynamics between basins of attraction of minima. Moreover we extract some information about the landscape itself, determining quantitatively few parameters describing it, such as the mean energy barrier value and the mean square distance between adjacent minima.

cond-mat.soft↗

arXiv2000

Topological Description of the Aging Dynamics in Simple Glasses

We numerically investigate the aging dynamics of a monatomic Lennard-Jones glass, focusing on the topology of the potential energy landscape which, to this aim, has been partitioned in basins of attraction of stationary points (saddles and minima). The analysis of the stationary points visited during the aging dynamics shows the existence of two distinct regimes: i) at short times, t t_c, the system mainly lies in basins pertaining to minima of slowly decreasing energy. The dynamics for t>t_c can be represented by a simple random walk on a network of minima with a jump probability proportional to the inverse of the waiting time.

cond-mat.dis-nn↗

arXiv2000

Saddles in the energy landscape probed by supercooled liquids

We numerically investigate the supercooled dynamics of two simple model liquids exploiting the partition of the multi-dimension configuration space in basins of attraction of the stationary points (inherent saddles) of the potential energy surface. We find that the inherent saddles order and potential energy are well defined functions of the temperature T. Moreover, decreasing T, the saddle order vanishes at the same temperature (T_MCT) where the inverse diffusivity appears to diverge as a power law. This allows a topological interpretation of T_MCT: it marks the transition from a dynamics between basins of saddles (T>T_MCT) to a dynamics between basins of minima (T<T_MCT).

cond-mat.dis-nn↗

arXiv2000

Intra-molecular origin of the fast relaxations observed in the Brillouin light scattering spectra of molecular glass-formers

The Brillouin light scattering spectra of the o-terphenyl single crystal are compared with those of the liquid and the glass phases. This shows: i) the direct evidence of a fast relaxation at 5 GHz in both the single crystal and the glass; ii) a similar temperature dependence for the attenuation of the longitudinal sound waves in the single crystal and the glass; and iii) the absence of coupling between the fast relaxation and the transverse acoustic waves. These results allow us to assign such a relaxation to the coupling between the longitudinal acoustic waves and intra-molecular vibrations, and therefore to exclude any relationship between it and the glass transition.

cond-mat.dis-nn↗

arXiv2000

Molecular dynamics simulation of the fragile glass former ortho-terphenyl: a flexible molecule model

We present a realistic model of the fragile glass former orthoterphenyl and the results of extensive molecular dynamics simulations in which we investigated its basic static and dynamic properties. In this model the internal molecular interactions between the three rigid phenyl rings are described by a set of force constants, including harmonic and anharmonic terms; the interactions among different molecules are described by Lennard-Jones site-site potentials. Self-diffusion properties are discussed in detail together with the temperature and momentum dependencies of the self-intermediate scattering function. The simulation data are compared with existing experimental results and with the main predictions of the Mode Coupling Theory.

cond-mat.dis-nn↗

arXiv2000

Off-Equilibrium Effective Temperature in Monatomic Lennard-Jones Glass

The off-equilibrium dynamics of a monatomic Lennard-Jones glass is investigated after sudden isothermal density jumps (crunch) from well equilibrated liquid configurations towards the glassy state. The generalized fluctuation-dissipation relation has been studied and the temperature dependence of the violation factor m is found in agreement with the one step replica symmetry breaking scenario, i.e. at low temperature m(T) is found proportional to T up to an off-equilibrium effective temperature T_eff, where m(T_eff)=1. We report T_eff as a function of the density and compare it with the glass transition temperatures T_g as determined by equilibrium calculations.

cond-mat.dis-nn↗

arXiv2000

Relaxation processes in harmonic glasses?

A relaxation process, with the associated phenomenology of sound attenuation and sound velocity dispersion, is found in a simulated harmonic Lennard-Jones glass. We propose to identify this process with the so called microscopic (or instantaneous) relaxation process observed in real glasses and supercooled liquids. A model based on the memory function approach accounts for the observation, and allows to relate to each others: 1) the characteristic time and strength of this process, 2) the low frequency limit of the dynamic structure factor of the glass, and 3) the high frequency sound attenuation coefficient, with its observed quadratic dependence on the momentum transfer.

cond-mat.dis-nn↗

arXiv1999

Non-dynamic origin of the acoustic attenuation at high frequency in glasses

The sound attenuation in the THz region is studied down to T=16 K in glassy glycerol by inelastic x-ray scattering. At striking variance with the decrease found below 100 K in the GHz data, the attenuation in the THz range does not show any T dependence. This result i) indicates the presence of two different attenuation mechanisms, active respectively in the high and low frequency limits; ii) demonstrates the non-dynamic origin of the attenuation of THz sound waves, and confirms a similar conclusion obtained in SiO2 glass by molecular dynamics; and iii) supports the low frequency attenuation mechanism proposed by Fabian and Allen (Phys.Rev.Lett. 82, 1478 (1999)).

cond-mat.dis-nn↗

arXiv1998

Elastic constant dishomogeneity and $Q^2$ dependence of the broadening of the dynamical structure factor in disordered systems

We propose an explanation for the quadratic dependence on the momentum $Q$, of the broadening of the acoustic excitation peak recently found in the study of the dynamic structure factor of many real and simulated glasses. We ascribe the observed $Q^2$ law to the spatial fluctuations of the local wavelength of the collective vibrational modes, in turn produced by the dishomegeneity of the inter-particle elastic constants. This explanation is analitically shown to hold for 1-dimensional disordered chains and satisfatorily numerically tested in both 1 and 3 dimensions.

cond-mat.dis-nn↗