Unifying different interpretations of the nonlinear response in glass-forming liquids.

This work aims at reconsidering several interpretations coexisting in the recent literature concerning nonlinear susceptibilities in supercooled liquids. We present experimental results on glycerol and propylene carbonate, showing that the three independent cubic susceptibilities have very similar frequency and temperature dependences, for both their amplitudes and phases. This strongly suggests a unique physical mechanism responsible for the growth of these nonlinear susceptibilities. We show that the framework proposed by two of us [J.-P. Bouchaud and G. Biroli, Phys. Rev. B 72, 064204 (2005)PRBMDO1098-012110.1103/PhysRevB.72.064204], where the growth of nonlinear susceptibilities is intimately related to the growth of glassy domains, accounts for all the salient experimental features. We then review several complementary and/or alternative models and show that the notion of cooperatively rearranging glassy domains is a key (implicit or explicit) ingredient to all of them. This paves the way for future experiments, which should deepen our understanding of glasses.

Fifth-order susceptibility unveils growth of thermodynamic amorphous order in glass-formers.

Glasses are ubiquitous in daily life and technology. However, the microscopic mechanisms generating this state of matter remain subject to debate: Glasses are considered either as merely hyperviscous liquids or as resulting from a genuine thermodynamic phase transition toward a rigid state. We show that third- and fifth-order susceptibilities provide a definite answer to this long-standing controversy. Performing the corresponding high-precision nonlinear dielectric experiments for supercooled glycerol and propylene carbonate, we find strong support for theories based on thermodynamic amorphous order. Moreover, when lowering temperature, we find that the growing transient domains are compact--that is, their fractal dimension d(f) = 3. The glass transition may thus represent a class of critical phenomena different from canonical second-order phase transitions for which d(f) < 3.

Level Statistics and Localization Transitions of Lévy Matrices.

This work provides a thorough study of Lévy, or heavy-tailed, random matrices (LMs). By analyzing the self-consistent equation on the probability distribution of the diagonal elements of the resolvent we establish the equation determining the localization transition and obtain the phase diagram. Using arguments based on supersymmetric field theory and Dyson Brownian motion we show that the eigenvalue statistics is the same one as of the Gaussian orthogonal ensemble in the whole delocalized phase and is Poisson-like in the localized phase. Our numerics confirm these findings, valid in the limit of infinitely large LMs, but also reveal that the characteristic scale governing finite size effects diverges much faster than a power law approaching the transition and is already very large far from it. This leads to a very wide crossover region in which the system looks as if it were in a mixed phase. Our results, together with the ones obtained previously, now provide a complete theory of Lévy matrices.

Ultrafast dynamics of fluctuations in high-temperature superconductors far from equilibrium.

Despite extensive work on high-temperature superconductors, the critical behavior of an incipient condensate has so far been studied exclusively under equilibrium conditions. Here, we excite Bi(2)Sr(2)CaCu(2)O(8+δ) with a femtosecond laser pulse and monitor the subsequent nonequilibrium dynamics of the midinfrared conductivity. Our data allow us to discriminate temperature regimes where superconductivity is either coherent, fluctuating or vanishingly small. Above the transition temperature T(c), we make the striking observation that the relaxation to equilibrium exhibits power-law dynamics and scaling behavior, both for optimally and underdoped superconductors. Our findings can in part be modeled using time-dependent Ginzburg-Landau theory, and they provide strong indication of universality in systems far from equilibrium.

Evidence of growing spatial correlations during the aging of glassy glycerol.

We have measured, as a function of the age t(a), the aging of the nonlinear dielectric susceptibility χ(3) of glycerol below the glass transition. Whereas the linear susceptibility can be accurately accounted for in terms of an age dependent relaxation time τ(α)(t(a)), this scaling breaks down for χ(3), suggesting an increase of the amplitude of χ(3). This is a strong indication that the number N(corr) of molecules involved in relaxation events increases with t(a). For T=0.96×T(g), we find that N(corr) increases by ~10% when t(a) varies from 1 to 100 ks. This sheds new light on the relation between length scales and time scales in glasses.

Evidence of growing spatial correlations at the glass transition from nonlinear response experiments.

The ac nonlinear dielectric response chi3(omega,T) of glycerol was measured close to its glass transition temperature T(g) to investigate the prediction that supercooled liquids respond in an increasingly nonlinear way as the dynamics slows down (as spin glasses do). We find that chi3(omega,T) indeed displays several nontrivial features. It is peaked as a function of the frequency omega and obeys scaling as a function of omega tau(T), with tau(T) the relaxation time of the liquid. The height of the peak, proportional to the number of dynamically correlated molecules N(corr)(T), increases as the system becomes glassy, and chi3 decays as a power law of omega over several decades beyond the peak. These findings confirm the collective nature of the glassy dynamics and provide the first direct estimate of the T dependence of N(corr).

Spatiotemporal hierarchy of relaxation events, dynamical heterogeneities, and structural reorganization in a supercooled liquid.

We identify the pattern of microscopic dynamical relaxation for a two-dimensional glass-forming liquid. On short time scales, bursts of irreversible particle motion, called cage jumps, aggregate into clusters. On larger time scales, clusters aggregate both spatially and temporally into avalanches. This propagation of mobility takes place along the soft regions of the systems, which have been identified by computing isoconfigurational Debye-Waller maps. Our results characterize the way in which dynamical heterogeneity evolves in moderately supercooled liquids and reveal that it is astonishingly similar to the one found for dense glassy granular media.

Building blocks of dynamical heterogeneities in dense granular media.

We investigate experimentally the connection between short time dynamics and long time dynamical heterogeneities within a dense granular media under cyclic shear. We show that dynamical heterogeneities result from a two time scales process. Short time but already collective events consisting in clustered cage jumps concentrate most of the nonaffine displacements. On larger time scales, such clusters appear aggregated both temporally and spatially in avalanches which eventually build the large scales dynamical heterogeneities. Our results indicate that facilitation plays an important role in the relaxation process although it does not appear to be conserved as proposed in many models studied in the literature.

Spatial correlations in the dynamics of glassforming liquids: experimental determination of their temperature dependence.

We use recently introduced three-point dynamic susceptibilities to obtain an experimental determination of the temperature evolution of the number of molecules Ncorr that are dynamically correlated during the structural relaxation of supercooled liquids. We first discuss in detail the physical content of three-point functions that relate the sensitivity of the averaged two-time dynamics to external control parameters (such as temperature or density), as well as their connection to the more standard four-point dynamic susceptibility associated with dynamical heterogeneities. We then demonstrate that these functions can be experimentally determined with good precision. We gather available data to obtain the temperature dependence of Ncorr for a large number of supercooled liquids over a wide range of relaxation time scales from the glass transition up to the onset of slow dynamics. We find that Ncorr systematically grows when approaching the glass transition. It does so in a modest manner close to the glass transition, which is consistent with an activation-based picture of the dynamics in glassforming materials. For higher temperatures, there appears to be a regime where Ncorr behaves as a power-law of the relaxation time. Finally, we find that the dynamic response to density, while being smaller than the dynamic response to temperature, behaves similarly, in agreement with theoretical expectations.

Spontaneous and induced dynamic fluctuations in glass formers. I. General results and dependence on ensemble and dynamics.

We study theoretically and numerically a family of multipoint dynamic susceptibilities that quantify the strength and characteristic length scales of dynamic heterogeneities in glass-forming materials. We use general theoretical arguments (fluctuation-dissipation relations and symmetries of relevant dynamical field theories) to relate the sensitivity of averaged two-time correlators to temperature and density to spontaneous fluctuations of the local dynamics. Our theoretical results are then compared to molecular dynamics simulations of the Newtonian, Brownian, and Monte Carlo dynamics of two representative glass-forming liquids, a fragile binary Lennard-Jones mixture, and a model for the strong glass-former silica. We justify in detail the claim made by Berthier et al. [Science 310, 1797 (2005)] that the temperature dependence of correlation functions allows one to extract useful information on dynamic length scales in glassy systems. We also discuss some subtle issues associated with the choice of microscopic dynamics and of statistical ensemble through conserved quantities, which are found to play an important role in determining dynamic correlations.

Spontaneous and induced dynamic correlations in glass formers. II. Model calculations and comparison to numerical simulations.

We study in detail the predictions of various theoretical approaches, in particular, mode-coupling theory (MCT) and kinetically constrained models (KCMs), concerning the time, temperature, and wave vector dependence of multipoint correlation functions that quantify the strength of both induced and spontaneous dynamical fluctuations. We also discuss the precise predictions of MCT concerning the statistical ensemble and microscopic dynamics dependence of these multipoint correlation functions. These predictions are compared to simulations of model fragile and strong glass-forming liquids. Overall, MCT fares quite well in the fragile case, in particular, explaining the observed crucial role of the statistical ensemble and microscopic dynamics, while MCT predictions do not seem to hold in the strong case. KCMs provide a simplified framework for understanding how these multipoint correlation functions may encode dynamic correlations in glassy materials. However, our analysis highlights important unresolved questions concerning the application of KCMs to supercooled liquids.

Direct experimental evidence of a growing length scale accompanying the glass transition.

Understanding glass formation is a challenge, because the existence of a true glass state, distinct from liquid and solid, remains elusive: Glasses are liquids that have become too viscous to flow. An old idea, as yet unproven experimentally, is that the dynamics becomes sluggish as the glass transition approaches, because increasingly larger regions of the material have to move simultaneously to allow flow. We introduce new multipoint dynamical susceptibilities to estimate quantitatively the size of these regions and provide direct experimental evidence that the glass formation of molecular liquids and colloidal suspensions is accompanied by growing dynamic correlation length scales.

Dynamical heterogeneity close to the jamming transition in a sheared granular material.

The dynamics of a bidimensional dense granular packing under cyclic shear is experimentally investigated close to the jamming transition. Measurement of multipoint correlation functions are produced. The self-intermediate scattering function, displaying slower than exponential relaxation, suggests dynamic heterogeneity. Further analysis of four point correlation functions reveal that the grain relaxations are strongly correlated and spatially heterogeneous, especially at the time scale of the collective rearrangements. Finally, a dynamical correlation length is extracted from a spatiotemporal pattern of mobility. Our experimental results open the way to a systematic study of dynamic correlation functions in granular materials.

Cluster dynamical mean field analysis of the mott transition.

We investigate the Mott transition using a cluster extension of dynamical mean field theory (DMFT). In the absence of frustration we find no evidence for a finite temperature Mott transition. Instead, in a frustrated model, we observe signatures of a finite temperature Mott critical point in agreement with experimental studies of kappa organics and with single-site DMFT. As the Mott transition is approached, a clear momentum dependence of the electron lifetime develops on the Fermi surface with the formation of cold regions along the diagonal direction of the Brillouin zone. Furthermore, the variation of the effective mass is no longer equal to the inverse of the quasiparticle residue, as in DMFT, and is reduced approaching the Mott transition.

Metastable states in glassy systems.

Truly stable metastable states are an artifact of the mean-field approximation or the zero-temperature limit. If such appealing concepts in glass theory as configurational entropy are to have a meaning beyond these approximations, one needs to cast them in a form involving states with finite lifetimes. Starting from elementary examples and using the results of Gaveau and Schulman, we propose a simple expression for the configurational entropy and revisit the question of taking flat averages over metastable states. The construction is applicable to finite-dimensional systems, and we explicitly show that for simple mean-field glass models it recovers, justifies, and generalizes the known results. The calculation emphasises the appearance of new dynamical order parameters.