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

How does the relaxation of a supercooled liquid depend on its microscopic dynamics?

Using molecular dynamics computer simulations we investigate how the relaxation dynamics of a simple supercooled liquid with Newtonian dynamics differs from the one with a stochastic dynamics. We find that, apart from the early beta-relaxation regime, the two dynamics give rise to the same relaxation behavior. The increase of the relaxation times of the system upon cooling, the details of the alpha-relaxation, as well as the wave vector dependence of the Edwards-Anderson-parameters are independent of the microscopic dynamics.Comment: 6 pages of Latex, 4 figure

Finite size effects in the dynamics of glass-forming liquids

We present a comprehensive theoretical study of finite size effects in the relaxation dynamics of glass-forming liquids. Our analysis is motivated by recent theoretical progress regarding the understanding of relevant correlation length scales in liquids approaching the glass transition. We obtain predictions both from general theoretical arguments and from a variety of specific perspectives: mode-coupling theory, kinetically constrained and defect models, and random first order transition theory. In the latter approach, we predict in particular a non-monotonic evolution of finite size effects across the mode-coupling crossover due to the competition between mode-coupling and activated relaxation. We study the role of competing relaxation mechanisms in giving rise to non-monotonic finite size effects by devising a kinetically constrained model where the proximity to the mode-coupling singularity can be continuously tuned by changing the lattice topology. We use our theoretical findings to interpret the results of extensive molecular dynamics studies of four model liquids with distinct structures and kinetic fragilities. While the less fragile model only displays modest finite size effects, we find a more significant size dependence evolving with temperature for more fragile models, such as Lennard-Jones particles and soft spheres. Finally, for a binary mixture of harmonic spheres we observe the predicted non-monotonic temperature evolution of finite size effects near the fitted mode-coupling singularity, suggesting that the crossover from mode-coupling to activated dynamics is more pronounced for this model. Finally, we discuss the close connection between our results and the recent report of a non-monotonic temperature evolution of a dynamic length scale near the mode-coupling crossover in harmonic spheres.Comment: 19 pages, 10 figures. V2: response to referees + refs added (close to published version

Fluctuation-dissipation relation in a sheared fluid

In a fluid out of equilibrium, the fluctuation dissipation theorem (FDT) is usually violated. Using molecular dynamics simulations, we study in detail the relationship between correlation and response functions in a fluid driven into a stationary non-equilibrium state. Both the high temperature fluid state and the low temperature glassy state are investigated. In the glassy state, the violation of the FDT is quantitatively identical to the one observed previously in an aging system in the absence of external drive. In the fluid state, violations of the FDT appear only when the fluid is driven beyond the linear response regime, and are then similar to those observed in the glassy state. These results are consistent with the picture obtained earlier from theoretical studies of driven mean-field disordered models, confirming the similarity between these models and real glasses.Comment: 4 pages, latex, 3 ps figure

Nearly-logarithmic decay in the colloidal hard-sphere system

Nearly-logarithmic decay is identified in the data for the mean-squared displacement of the colloidal hard-sphere system at the liquid-glass transition [v. Megen et. al, Phys. Rev. E 58, 6073(1998)]. The solutions of mode-coupling theory for the microscopic equations of motion fit the experimental data well. Based on these equations, the nearly-logarithmic decay is explained as the equivalent of a beta-peak phenomenon, a manifestation of the critical relaxation when the coupling between of the probe variable and the density fluctuations is strong. In an asymptotic expansion, a Cole-Cole formula including corrections is derived from the microscopic equations of motion, which describes the experimental data for three decades in time.Comment: 4 pages, 3 figure

Crossovers in the dynamics of supercooled liquids probed by an amorphous wall

We study the relaxation dynamics of a binary Lennard-Jones liquid in the presence of an amorphous wall generated from equilibrium particle configurations. In qualitative agreement with the results presented in Nature Phys. {\bf 8}, 164 (2012) for a liquid of harmonic spheres, we find that our binary mixture shows a saturation of the dynamical length scale close to the mode-coupling temperature $T_c$. Furthermore we show that, due to the broken symmetry imposed by the wall, signatures of an additional change in dynamics become apparent at a temperature well above $T_c$. We provide evidence that this modification in the relaxation dynamics occurs at a recently proposed dynamical crossover temperature $T_s > T_c$, which is related to the breakdown of the Stokes-Einstein relation. We find that this dynamical crossover at $T_s$ is also observed for a system of harmonic spheres as well as a WCA liquid, showing that it may be a general feature of glass-forming systems.Comment: 10 pages, 8 figure

Coupling/decoupling between translational and rotational dynamics in a supercooled molecular liquid

We use molecular dynamics computer simulations to investigate the coupling/decoupling between translational and rotational dynamics in a glass-forming liquid of dumbbells. This is done via a careful analysis of the $\alpha$-relaxation time $\tau_{q^{*}}^{\rm C}$ of the incoherent center-of-mass density correlator at the structure factor peak, the $\alpha$-relaxation time $\tau_{2}$ of the reorientational correlator, and the translational ($D_{t}$) and rotational ($D_{r}$) diffusion constants. We find that the coupling between the relaxation times $\tau_{q^{*}}^{\rm C}$ and $\tau_{2}$ increases with decreasing temperature $T$, whereas the coupling decreases between the diffusivities $D_{t}$ and $D_{r}$. In addition, the $T$-dependence of $D_{t}$ decouples from that of $1/\tau_{2}$, which is consistent with previous experiments and has been interpreted as a signature of the "translation-rotation decoupling." We trace back these apparently contradicting observations to the dynamical heterogeneities in the system. We show that the decreasing coupling in the diffusivities $D_{t}$ and $D_{r}$ is only apparent due to the inadequacy of the concept of the rotational diffusion constant for describing the reorientational dynamics in the supercooled state. We also argue that the coupling between $\tau_{q^{*}}^{\rm C}$ and $\tau_{2}$ and the decoupling between $D_{t}$ and $1/\tau_{2}$, both of which strengthen upon cooling, can be consistently understood in terms of the growing dynamic length scale.Comment: revised manuscript, to appear in Phys. Rev. Let

Growing spatial correlations of particle displacements in a simulated liquid on cooling toward the glass transition

We define a correlation function that quantifies the spatial correlation of single-particle displacements in liquids and amorphous materials. We show for an equilibrium liquid that this function is related to fluctuations in a bulk dynamical variable. We evaluate this function using computer simulations of an equilibrium glass-forming liquid, and show that long range spatial correlations of displacements emerge and grow on cooling toward the mode coupling critical temperature

Dynamics in a supercooled liquid of symmetric dumbbells: Reorientational hopping for small molecular elongations

We present extensive molecular dynamics simulations of a liquid of symmetric dumbbells, for constant packing fraction, as a function of temperature and molecular elongation. For large elongations, translational and rotational degrees of freedom freeze at the same temperature. For small elongations only the even rotational degrees of freedom remain coupled to translational motions and arrest at a finite common temperature. The odd rotational degrees of freedom remain ergodic at all investigated temperature and the temperature dependence of the corresponding characteristic time is well described by an Arrhenius law. Finally, we discuss the evidence in favor of the presence of a type-A transition temperature for the odd rotational degrees of freedom, distinct from the type-B transition associated with the arrest of the translational and even rotational ones, as predicted by the mode-coupling theory for the glass transition.Comment: 4 pages, 3 figure