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The dynamic structure factor, S(Q,w), of vitreous silica, has been measured by inelastic X-ray scattering in the exchanged wavevector (Q) region Q=4-16.5 nm-1 and up to energies hw=115 meV in the Stokes side. The unprecedented statistical accuracy in such an extended energy range allows to accurately determine the longitudinal current spectra, and the energies of the vibrational excitations. The simultaneous observation of two excitations in the acoustic region, and the persistence of propagating sound waves up to Q values comparable with the (pseudo-)Brillouin zone edge, allow to observe a positive dispersion in the generalized sound velocity that, around Q=5 nm-1, varies from 6500 to 9000 m/s: this phenomenon was never experimentally observed in a glass., Comment: 5 pages, 3 figures. To appear in Phys. Rev. B

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 figures

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.

The concept of fragility provides a possibility to rank different supercooled liquids on the basis of the temperature dependence of dynamic and/or thermodynamic quantities. We recall here the definitions of kinetic and thermodynamic fragility proposed in the last years and discuss their interrelations. At the same time we analyze some recently introduced models for the statistical properties of the potential energy landscape. Building on the Adam-Gibbs relation, which connects structural relaxation times to configurational entropy, we analyze the relation between statistical properties of the landscape and fragility. We call attention to the fact that the knowledge of number, energy depth and shape of the basins of the potential energy landscape may not be sufficient for predicting fragility. Finally, we discuss two different possibilities for generating strong behavior., Comment: 17 pages, 10 figures; accepted version, minor corrections

The high frequency collective dynamics of molten potassium has been investigated by inelastic x-ray scattering, disclosing an energy/momentum transfer region unreachable by previous neutron scattering experiments (INS). We find that a two-step relaxation scenario, similar to that found in other liquid metals, applies to liquid potassium. In particular, we show how the sound velocity determined by INS experiments, exceeding the hydrodynamic value by $\approx 30 %$, is the higher limit of a speed up, located in the momentum region $1

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

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 figures

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., Comment: 9 pages, 11 figures

Features of the energy landscape sampled by supercooled liquids are numerically analyzed for several Lennard-Jones like model systems. The properties of quasisaddles (minima of the square gradient of potential energy W=|grad V|^2), are shown to have a direct relationship with the dynamical behavior, confirming that the quasisaddle order extrapolates to zero at the mode-coupling temperature T_MCT. The same result is obtained either analyzing all the minima of W or the saddles (absolute minima of W), supporting the conjectured similarity between quasisaddles and saddles, as far as the temperature dependence of the properties influencing the slow dynamics is concerned. We find evidence of universality in the shape of the landscape: plots for different systems superimpose into master curves, once energies and temperatures are scaled by T_MCT. This allows to establish a quantitative relationship between T_MCT and potential energy barriers for LJ-like systems, and suggests a possible generalization to different model liquids., Comment: 8 pages, 5 figures

We analyze the dynamics and the geometric properties of the Potential Energy Surfaces (PES) of the k-Trigonometric Model (kTM), defined by a fully-connected k-body interaction. This model has no thermodynamic transition for k=1, a second order one for k=2, and a first order one for k>2. In this paper we i) show that the single particle dynamics can be traced back to an effective dynamical system (with only one degree of freedom); ii) compute the diffusion constant analytically; iii) determine analytically several properties of the self correlation functions apart from the relaxation times which we calculate numerically; iv) relate the collective correlation functions to the ones of the effective degree of freedom using an exact Dyson-like equation; v) using two analytical methods, calculate the saddles of the PES that are visited by the system evolving at fixed temperature. On the one hand we minimize |grad V|^2, as usually done in the numerical study of supercooled liquids and, on the other hand, we compute the saddles with minimum distance (in configuration space) from initial equilibrium configurations. We find the same result from the two calculations and we speculate that the coincidence might go beyond the specific model investigated here., Comment: 36 pages, 13 figures

The potential energy landscape in the Kob-Andersen Lennard-Jones binary mixture model has been studied carefully from liquid down to the supercooled regime, from T =2 down to T =0.46. One thousand of independent configurations along the time evolution have been examined at each investigated temperature. From the starting configuration we searched the nearest saddle (or quasi-saddle) and minimum of the potential energy. The vibrational densities of states for the starting and the two derived configurations have been evaluated. Besides the number of negative eigenvalues of saddle, other quantities show some signature of the approaching of the dynamical arrest temperature., Comment: 15 pages, 8 figures, to be published on Journal of Physics: Cond. Matt

We use the saddle-approach, recently introduced in the numerical investigation of simple model liquids, in the analysis of a mean-field solvable system. The investigated system is the k-trigonometric model, a k-body interaction mean field system, that generalizes the trigonometric model introduced by Madan and Keyes [J. Chem. Phys. 98, 3342 (1993)] and that has been recently introduced to investigate the relationship between thermodynamics and topology of the configuration space. We find a close relationship between the properties of saddles (stationary points of the potential energy surface) visited by the system and the dynamics. In particular the temperature dependence of saddle order follows that of the diffusivity, both having an Arrhenius behavior at low temperature and a similar shape in the whole temperature range. Our results confirm the general usefulness of the saddle-approach in the interpretation of dynamical processes taking place in interacting systems., Comment: 7 pages, 8 figures

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., Comment: to be published in PRE Rapid Commun

We present a numerical simulation study of the density-dependence (rho = 2.2 - 4.0 g/cm^3) of the high-energy collective dynamics in vitreous silica at mesoscopic wavevectors (Q = 1 - 18 nm^-1). The density-dependence of the longitudinal and transverse current spectra provides evidence that the excess modes observed in the density of states of this and many other glasses, i.e. the Boson Peak, arises from the high-Q limit of the quasi-transverse acoustic branch. This conclusion emerges from the comparison of the numerical results with the experimentally observed energy-shift and intensity variation of the Boson Peak with increasing density., Comment: 8 pages, 4 figures

The microscopic dynamics in liquid gallium (l-Ga) at melting (T=315 K) has been studied by inelastic x-ray scattering. We demonstrate the existence of collective acoustic-like modes up to wave-vectors above one half of the first maximum of the static structure factor, at variance with earlier results from inelastic neutron scattering data [F.J. Bermejo et al. Phys. Rev. E 49, 3133 (1994)]. Despite the structural (an extremely rich polymorphism and rather complex phase diagram) and electronic (mixed valence) peculiarity of l-Ga, its collective dynamics is strikingly similar to the one of Van der Walls and alkali metals liquids. This result speaks in favor of the universality of the short time dynamics in monatomic liquids rather than of system-specific dynamics., Comment: LaTex format, 11 pages, 4 EncapsulatedPostScript figures

We report a molecular dynamics (MD) study of the collective dynamics of a simple monatomic liquid -interacting through a two body potential that mimics that of lithium- across the liquid-glass transition. In the glassy phase we find evidences of a fast relaxation process similar to that recently found in Lennard-Jones glasses. The origin of this process is ascribed to the topological disorder, i.e. to the dephasing of the different momentum $Q$ Fourier components of the actual normal modes of vibration of the disordered structure. More important, we find that the fast relaxation persists in the liquid phase with almost no temperature dependence of its characteristic parameters (strength and relaxation time). We conclude, therefore, that in the liquid phase well above the melting point, at variance with the usual assumption of {\it un-correlated} binary collisions, the short time particles motion is strongly {\it correlated} and can be described via a normal mode expansion of the atomic dynamics., Comment: 7 pages, 7 .eps figs. To appear in Phys. Rev. E

Inelastic X-ray Scattering measurements of the dynamics structure factor have bene performed on vitreous Beryllium Fluoride ({\it v-}BeF$_2$) at $T$=297 K in the momentum transfer, $Q$, range $Q$=1.5$\div$10 nm$^{-1}$. We find evidence of well defined high frequency acoustic modes. The energy position and linewidth of the excitations disperse with $Q$ as $\propto Q$ and $\propto Q^2$, respectively up to about one half of the first maximum of the static structure factor. Their magnitude compare favorably with low-frequency sound velocity and absorption data. The results indicate worth mentioning similarities of the high frequency collective dynamics of different network forming glasses such as {\it v-}B$_2$O$_3$ and {\it v-}SiO$_2$., Comment: 17 pages, 5 .ps figs

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$\div$23 nm$^{-1}$ and in the temperature range 80$\div$570 K. Beside the propagating longitudinal excitations modes, at low temperature the spectra show a second non $Q$-dispersing peak at $\hbar \Omega_T$$\approx$8.5 meV. We assign this peak to the transverse dynamics that, in topologically disordered systems, acquires a longitudinal symmetry component. This assignment is substantiated by the observation that, in the liquid, this peak vanishes when the structural relaxation time $\tau_\alpha$ approaches $\Omega_T^{-1}$, a behavior consistent with the condition $\tau_\alpha \Omega_T^{-1}$$>>$1 required for the existence of a transverse-like dynamics in the liquid state., Comment: 13 pages, 5 PostScript figures

We show that the presence and the location of first order phase transitions in a thermodynamic system can be deduced by the study of the topology of the potential energy function, V(q), without introducing any thermodynamic measure. In particular, we present the thermodynamics of an analytically solvable mean-field model with a k-body interaction which -depending on the value of k- displays no transition (k=1), second order (k=2) or first order (k>2) phase transition. This rich behavior is quantitatively retrieved by the investigation of a topological invariant, the Euler characteristic, of some submanifolds of the configuration space. Finally, we conjecture a direct link between the Euler characteristic and the thermodynamic entropy., Comment: 6 pages, 2 figures

We present a numerical simulation study of a simple monatomic Lennard-Jones liquid under shear flow, as a function of both temperature and shear rate. By investigating different observables we find that i) It exists a line in the (temperature-shear) plane that sharply marks the boarder between an ``equilibrium'' and a ``shear-controlled'' region for both the dynamic and the thermodynamic quantities; and ii) Along this line the structural relaxation time, is proportional to the inverse shear rate, i.e. to the typical time-scale introduced by the shear flow. Above the line the liquid dynamics is unaffected by the shear flow, while below it both temperature and shear rate control the particle motion., Comment: 14 pages, 5 figures

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., Comment: To be published in J. Chem. Phys

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 figures

Inelastic X-ray scattering data have been collected for liquid sodium at T=390 K, i.e. slightly above the melting point. Owing to the very high instrumental resolution, pushed up to 1.5 meV, it has been possible to determine accurately the dynamic structure factor, $S(Q,\omega)$, in a wide wavevector range, $1.5 \div 15$ nm$^{-1}$, and to investigate on the dynamical processes underlying the collective dynamics. A detailed analysis of the lineshape of $S(Q,\omega)$, similarly to other liquid metals, reveals the co-existence of two different relaxation processes with slow and fast characteristic timescales respectively. The present data lead to the conclusion that: i) the picture of the relaxation mechanism based on a simple viscoelastic model fails; ii) although the comparison with other liquid metals reveals similar behavior, the data do not exhibit an exact scaling law as the principle of corresponding state would predict., Comment: RevTex, 7 pages, 6 eps figures. Accepted by Phys. Rev. E

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., Comment: 8th International Workshop on Disordered Systems, Andalo (Trento), Italy, March 2001

We study the interaction of the relaxation processes with the density fluctuations by molecular dynamics simulation of a flexible molecule model for o-terphenyl (oTP) in the liquid and supercooled phases. We find evidence, besides the structural relaxation, of a secondary vibrational relaxation whose characteristic time, few ps, is slightly temperature dependent. This i) confirms the result by Monaco et al. [Phys. Rev, E 62, 7595 (2000)] of the vibrational nature of the fast relaxation observed in Brillouin Light Scattering (BLS) experiments in oTP; and ii) poses a caveat on the interpretation of the BLS spectra of molecular systems in terms of a purely center of mass dynamics., Comment: RevTeX, 5 pages, 4 eps figures

Using a realistic flexible molecule model of the fragile glass former orthoterphenyl, we calculate via molecular dynamics simulation the collective dynamic structure factor, recently measured in this system by Inelastic X-ray Scattering. The comparison of the simulated and measured dynamic structure factor, and the study of its properties in an extended momentum, frequency and temperature range allows: i) to conclude that the utilized molecular model gives rise to a dynamic structure factor in agreement with the experimental data, for those thermodynamic states and momentum values where the latter are available; ii) to confirm the existence of a slope discontinuity on the T-dependence of the sound velocity that, at finite Q, takes place at a temperature T_x higher than the calorimetric glass transition temperature T_g; iii) to find that the values of T_x is Q-dependent and that its vanishing Q limit is consistent with T_g. The latter finding is interpreted within the framework of the current description of the dynamics of supercooled liquids in terms of exploration of the potential energy landscape., Comment: RevTex, 9 pages, 10 eps figures

We present a molecular dynamics study of the collective dynamics of a flexible model for the fragile glass-former orthoterphenyl [ S. Mossa, R. Di leonardo, G. Ruocco, and M. Sampoli, Phys. Rev. E 62, 612 (2000)]. We study the behavior of the coherent scattering functions, considering the density fluctuations of both molecular and phenyl rings centers of mass; moreover we directly simulate the neutron scattering spectra taking into account both the contributions due to the carbon and hydrogens atoms. We compare our results with the main predictions of the Mode Coupling Theory and with the available coherent neutron scattering experimental data., Comment: 13 pages, 15 eps figures

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, tt_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., Comment: 4 pages, 5 postscript figures

New inelastic X-ray scattering experiments have been performed on liquid lithium in a wide wavevector range. With respect to the previous measurements, the instrumental resolution, improved up to 1.5 meV, allows to accurately investigate the dynamical processes determining the observed shape of the the dynamic structure factor, $S(Q,\omega)$. A detailed analysis of the lineshapes shows the co-existence of relaxation processes with both a slow and a fast characteristic timescales, and therefore that pictures of the relaxation mechanisms based on a simple viscoelastic model must be abandoned., Comment: 5 pages, 4 .PS figures

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., Comment: 4 Pages, 4 Figures

An inelastic X-ray scattering experiment has been performed in liquid aluminum with the purpose of studying the collective excitations at wavevectors below the first sharp diffraction peak. The high instrumental resolution (up to 1.5 meV) allows an accurate investigation of the dynamical processes in this liquid metal on the basis of a generalized hydrodynamics framework. The outcoming results confirm the presence of a viscosity relaxation scenario ruled by a two timescale mechanism, as recently found in liquid lithium., Comment: 8 pages, 7 figures

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

The dynamical structure factor (S(Q,E)) of vitreous silica has been measured by Inelastic X-ray Scattering varying the exchanged wavevector (Q) at fixed exchanged energy (E) - an experimental procedure that, contrary to the usual one at constant Q, provides spectra with much better identified inelastic features. This allows the first direct evidence of Brillouin peaks in the S(Q,E) of SiO_2 at energies above the Boson Peak (BP) energy, a finding that excludes the possibility that the BP marks the transition from propagating to localised dynamics in glasses., Comment: 4 pages, 3 Postscript figures. To appear in Physical Review Letters

Three classes of harmonic disorder systems (Lennard-Jones like glasses, percolators above threshold, and spring disordered lattices) have been numerically investigated in order to clarify the effect of different types of disorder on the mechanism of high frequency sound attenuation. We introduce the concept of frustration in structural glasses as a measure of the internal stress, and find a strong correlation between the degree of frustration and the exponent alpha that characterizes the momentum dependence of the sound attenuation $Gamma(Q)$$\simeq$$Q^\alpha$. In particular, alpha decreases from about d+1 in low-frustration systems (where d is the spectral dimension), to about 2 for high frustration systems like the realistic glasses examined., Comment: Revtex, 4 pages including 4 figures

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., Comment: 4 pages,4 figures

New inelastic X-ray scattering experiments have been performed in liquid lithium at two different temperatures: T=475 K (slightly above the melting point) and 600 K. Taking advantage of the absence of any kinematical restriction and incoherent contribution, and pushing the instrumental resolution up to 1.5 meV, it was possible to perform an accurate investigation of the dynamic structure factor S(Q,E) in the wavevector range from 1 to 110 nm^-1. For Q smaller than Q_m=25 nm^-1, the position of the main peak of the static structure factor, a detailed analysis of the lineshapes shows that any picture of the relaxation mechanisms based on a simple viscoelastic model must be abandoned. All the spectral features can instead satisfactorily be accounted for by including both fast and slow relaxation processes. The physical origin of the slow relaxation is associated to the structural rearrangement, while the local nature of the fast one is extensively discussed. At larger Q values a gradual crossover from the strongly correlated to single particle dynamics occurs, with an important weight provided by quantum effects., Comment: 25 pages, 12 PS figures

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., Comment: 11 pages, 3 figures

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., Comment: 20 pages and 28 postscript figures

New Raman and incoherent neutron scattering data at various temperatures and molecular dynamic simulations in amorphous silica, are compared to obtain the Raman coupling coefficient $C(\omega)$ and, in particular, its low frequency limit. This study indicates that in the $\omega \to 0$ limit $C(\omega)$ extrapolates to a non vanishing value, giving important indications on the characteristics of the vibrational modes in disordered materials; in particular our results indicate that even in the limit of very long wavelength the local disorder implies non-regular local atomic displacements., Comment: Revtex, 4 ps figures

The dynamic structure factor, S(Q,E), of liquid lithium (T=475 K) has been determined by inelastic x-ray scattering (IXS) in the momentum transfer region (Q = 1.4-110 nm-1). These data allow to observe how, in a simple liquid, a phonon-like collective mode evolves towards the single particle dynamics. As a function of Q, one finds: i) at low Q's, a sound mode with a positive dispersion of the sound velocity, ii) at intermediate Q's, excitations whose energy oscillates similarly to phonons in the crystal Brillouin zones, and iii) at high Q's, the S(Q,E) approaches a Gaussian shape, indicating that the single particle dynamics has been reached., Comment: 3 pages and 5 figures

New temperature dependent inelastic x-ray (IXS) and Raman (RS) scattering data are compared to each other and with existing inelastic neutron scattering data in vitreous silica (v-SiO_2), in the 300 - 1775 K region. The IXS data show collective propagating excitations up to Q=3.5 nm^-1. The temperature behaviour of the excitations at Q=1.6 nm^-1 matches that of the boson peak found in INS and RS. This supports the acoustic origin of the excess of vibrational states giving rise to the boson peak in this glass., Comment: 10 pages and 4 figures

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))., Comment: 3 pages, 5 Figures, To be published in PRL

We analyze the properties of a Lennard-Jones system at the level of the potential energy landscape. After an exhaustive investigation of the topological features of the landscape of the systems, obtained studying small size sample, we describe the dynamics of the systems in the multi-dimensional configurational space by a simple model. This consider the configurational space as a connected network of minima where the dynamics proceeds by jumps described by an appropriate master equation. Using this model we are able to reproduce the long time dynamics and the low temperature regime. We investigate both the equilibrium regime and the off-equilibrium one, finding those typical glassy behavior usually observed in the experiments such as: {\it i)} stretched exponential relaxation, {\it ii)} temperature-dependent stretching parameter, {\it iii)} breakdown of the Stokes-Einstein relation, and {\it iv)} appearance of a critical temperature below which one observes deviation from the fluctuation-dissipation relation as consequence of the lack of equilibrium in the system., Comment: 11 pages (Latex), 9 ps figures

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., Comment: 4 pages, RevTeX, 5 postscript figures

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 figures

We develop an efficient numerical algorithm for the identification of a large number of saddle points of the potential energy function of Lennard- Jones clusters. Knowledge of the saddle points allows us to find many thousand adjacent minima of clusters containing up to 80 argon atoms and to locate many pairs of minima with the right characteristics to form two-level systems (TLS). The true TLS are singled out by calculating the ground-state tunneling splitting. The entropic contribution to all barriers is evaluated and discussed., Comment: 4 pages, RevTex, 2 PostScript figures

We report a molecular dynamics simulation study of the sound waves in vitreous silica in the mesoscopic exchanged momentum range. The calculated dynamical structure factors are in quantitative agreement with recent experimental inelastic neutron and x-ray scattering data. The analysis of the longitudinal and transverse current spectra allows to discriminate between opposite interpretations of the existing experimental data in favour of the propagating nature of the high frequency sound waves., Comment: 4 pages, Revtex, 4 ps figures; to be published in Phys. Rev. Lett., February 1988

The Raman coupling coefficients of site- and bond-percolators at concentration higher than percolation threshold are computed for two scattering mechanisms: Bond Polarizability (BPOL) and Dipole-Induced-Dipole (DID). The results show that DID does not follow a scaling law at low frequency, while in the case of BPOL the situation is less clear. The numerically computed frequency dependence in the case of BPOL, which can be considered a good scattering mechanism for a wide class of real glasses, is in semiquantitative agreement with experimental results., Comment: 10 pages, Revtex, 3 figures available from the authors, submitted to Physica A

Anelastic light scattering is computed numerically for model disordered systems (linear chains and 2-dimensional site and bond percolators), with and without electrical disorder. A detailed analysis of the vibrational modes and of their Raman activity evidences that two extreme mechanisms for scattering may be singled out. One of these resembles scattering from finite size systems, while the other mechanisms originates from spatial fluctuations of the polarizability and is such that modes in even small frequency intervals may have very different Raman activities. As a consequence, the average coupling coefficient $C(\omega)$ is the variance of a zero-average quantity. Our analysis shows that for both linear chains and 2-dimensional percolators the second mechanism dominates over the first, and therefore Raman scattering from disordered systems is essentially due to spatial fluctuations., Comment: 12 pages, Latex, 7 figures available on request.

The frequency dependence of the Raman coupling coefficient $C(\omega)$ is calculated numerically for square and cubic percolation clusters. No general scaling law in terms of the macroscopic parameters such as the fractal dimension $D$ or the spectral dimension $\overline d$ is found. $C(\omega)$ is sensitive to the microscopic structure of the clusters and depends on: site- or bond-percolation, presence or absence of dangling bonds, scattering mechanism and polarization, presence or absence of polarizability disorder. This situation makes the derivation of macroscopic parameters from Raman experiments unreliable., Comment: 4 pages revtex, 4 figures upon request, UTF-OS-301092