Structural Relaxation and Mode Coupling in a Simple Liquid: Depolarized Light Scattering in Benzene

We have measured depolarized light scattering in liquid benzene over the whole accessible temperature range and over four decades in frequency. Between 40 and 180 GHz we find a susceptibility peak due to structural relaxation. This peak shows stretching and time-temperature scaling as known from $\alpha$ relaxation in glass-forming materials. A simple mode-coupling model provides consistent fits of the entire data set. We conclude that structural relaxation in simple liquids and $\alpha$ relaxation in glass-forming materials are physically the same. A deeper understanding of simple liquids is reached by applying concepts that were originally developed in the context of glass-transition research.Comment: submitted to New J. Phy

Critical Decay at Higher-Order Glass-Transition Singularities

Within the mode-coupling theory for the evolution of structural relaxation in glass-forming systems, it is shown that the correlation functions for density fluctuations for states at A_3- and A_4-glass-transition singularities can be presented as an asymptotic series in increasing inverse powers of the logarithm of the time t: $\phi(t)-f\propto \sum_i g_i(x)$, where $g_n(x)=p_n(\ln x)/x^n$ with p_n denoting some polynomial and x=ln (t/t_0). The results are demonstrated for schematic models describing the system by solely one or two correlators and also for a colloid model with a square-well-interaction potential.Comment: 26 pages, 7 figures, Proceedings of "Structural Arrest Transitions in Colloidal Systems with Short-Range Attractions", Messina, Italy, December 2003 (submitted

Universal and non-universal features of glassy relaxation in propylene carbonate

It is demonstrated that the susceptibility spectra of supercooled propylene carbonate as measured by depolarized-light-scattering, dielectric-loss, and incoherent quasi-elastic neutron-scattering spectroscopy within the GHz window are simultaneously described by the solutions of a two-component schematic model of the mode-coupling theory (MCT) for the evolution of glassy dynamics. It is shown that the universal beta-relaxation-scaling laws, dealing with the asymptotic behavior of the MCT solutions, describe the qualitative features of the calculated spectra. But the non-universal corrections to the scaling laws render it impossible to achieve a complete quantitative description using only the leading-order-asymptotic results.Comment: 37 pages, 16 figures, to be published in Phys. Rev.

A quantitative test of the mode-coupling theory of the ideal glass transition for a binary Lennard-Jones system

Using a molecular dynamics computer simulation we determine the temperature dependence of the partial structure factors for a binary Lennard-Jones system. These structure factors are used as input data to solve numerically the wave-vector dependent mode-coupling equations in the long time limit. Using the so determined solutions, we compare the predictions of mode-coupling theory (MCT) with the results of a previously done molecular dynamics computer simulation [Phys. Rev. E 51, 4626 (1995), ibid. 52, 4134 (1995)]. From this comparison we conclude that MCT gives a fair estimate of the critical coupling constant, a good estimate of the exponent parameter, predicts the wave-vector dependence of the various nonergodicity parameters very well, except for very large wave-vectors, and gives also a very good description of the space dependence of the various critical amplitudes. In an attempt to correct for some of the remaining discrepancies between the theory and the results of the simulation, we investigate two small (ad hoc) modifications of the theory. We find that one modification gives a worse agreement between theory and simulation, whereas the second one leads to an improved agreement.Comment: Figures available from W. Ko

Cooperativity Beyond Caging: Generalized Mode Coupling Theory

The validity of mode coupling theory (MCT) is restricted by an uncontrolled factorization approximation of density correlations. The factorization can be delayed and ultimately avoided, however, by explicitly including higher order correlations. We explore this approach within a microscopically motivated schematic model. Analytic tractability allows us to discuss in great detail the impact of factorization at arbitrary order, including the limit of avoided factorization. Our results indicate a coherent picture for the capabilities as well as limitations of MCT. Moreover, including higher order correlations systematically defers the transition and ultimately restores ergodicity. Power-law divergence of the relaxation time is then replaced by continuous but exponential growth.Comment: 4 pages, 2 figure

Multiple-scattering effects on incoherent neutron scattering in glasses and viscous liquids

Incoherent neutron scattering experiments are simulated for simple dynamic models: a glass (with a smooth distribution of harmonic vibrations) and a viscous liquid (described by schematic mode-coupling equations). In most situations multiple scattering has little influence upon spectral distributions, but it completely distorts the wavenumber-dependent amplitudes. This explains an anomaly observed in recent experiments

Role of structural relaxations and vibrational excitations in the high-frequency dynamics of liquids and glasses

We present theoretical investigation on the high-frequency collective dynamics in liquids and glasses at microscopic length scales and terahertz frequency region based on the mode-coupling theory for ideal liquid-glass transition. We focus on recently investigated issues from inelastic-X-ray-scattering and computer-simulation studies for dynamic structure factors and longitudinal and transversal current spectra: the anomalous dispersion of the high-frequency sound velocity and the nature of the low-frequency excitation called the boson peak. It will be discussed how the sound mode interferes with other low-lying modes present in the system. Thereby, we provide a systematic explanation of the anomalous sound-velocity dispersion in systems -- ranging from high temperature liquid down to deep inside the glass state -- in terms of the contributions from the structural-relaxation processes and from vibrational excitations called the anomalous-oscillation peak (AOP). A possibility of observing negative dispersion -- the {\em decrease} of the sound velocity upon increase of the wave number -- is argued when the sound-velocity dispersion is dominated by the contribution from the vibrational dynamics. We also show that the low-frequency excitation, observable in both of the glass-state longitudinal and transversal current spectra at the same resonance frequency, is the manifestation of the AOP. As a consequence of the presence of the AOP in the transversal current spectra, it is predicted that the transversal sound velocity also exhibits the anomalous dispersion. These results of the theory are demonstrated for a model of the Lennard-Jones system.Comment: 25 pages, 22 figure

Spatial correlations in sheared isothermal liquids : From elastic particles to granular particles

Spatial correlations for sheared isothermal elastic liquids and granular liquids are theoretically investigated. Using the generalized fluctuating hydrodynamics, correlation functions for both the microscopic scale and the macroscopic scale are obtained. The existence of the long-range correlation functions obeying power laws has been confirmed. The validity of our theoretical predictions have been verified from the molecular dynamics simulation.Comment: 34 pages, 12 figure

Colloidal gelation and non-ergodicity transitions

Within the framework of the mode coupling theory (MCT) of structural relaxation, mechanisms and properties of non-ergodicity transitions in rather dilute suspensions of colloidal particles characterized by strong short-ranged attractions are studied. Results building on the virial expansion for particles with hard cores and interacting via an attractive square well potential are presented, and their relevance to colloidal gelation is discussed.Comment: 10 pages, 4 figures; Talk at the Conference: "Unifying Concepts in Glass Physics" ICTP Trieste, September 1999; to be published in J. Phys.: Condens. Matte

The mean-squared displacement of a molecule moving in a glassy system

The mean-squared displacement (MSD) of a hard sphere and of a dumbbell molecule consisting of two fused hard spheres immersed in a dense hard-sphere system is calculated within the mode-coupling theory for ideal liquid-glass transitions. It is proven that the velocity correlator, which is the second time derivative of the MSD, is the negative of a completely monotone function for times within the structural-relaxation regime. The MSD is found to exhibit a large time interval for structural relaxation prior to the onset of the $\alpha$-process which cannot be described by the asymptotic formulas for the mode-coupling-theory-bifurcation dynamics. The $\alpha$-process for molecules with a large elongation is shown to exhibit an anomalously wide cross-over interval between the end of the von-Schweidler decay and the beginning of normal diffusion. The diffusivity of the molecule is predicted to vary non-monotonically as function of its elongation.Comment: 18 pages, 12 figures, Phys. Rev. E, in prin