Takeshi Kawasaki, Takeaki Araki, Hajime Tanaka
This is our reply to the comment by Sausset and Tarjus (arXiv:0802.1631) on our paper titled "Correlation between Dynamic Heterogeneity and Medium-Range Order in Two-Dimensional Glass-Forming Liquids" [Phys. Rev. Lett. Vol. 99, No. 21, 215701 (2007)].
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This is a reply to cond-mat/0010033 by Newman and Stein, which is a comment on on our paper Phys. Rev. Lett. 85, 3017 (2000), cond-mat/0002134.
Reply to the Comment by L. Berthier and J.-P. Bouchaud, Phys. Rev. Lett. 90, 059701 (2003), also cond-mat/0209165, on our paper Phys. Rev. Lett. 89, 097201 (2002), also cond-mat/0203444
This is a Reply to the Comment of Muessel and Rieger cond-mat/9804063 to out paper on ``Aging Effects in a Lennerd-Jones Glass''. We show that the scaling function proposed by Muessel and Rieger does not lead to a satisfactory scaling of our aging data.
In his Comment, Krakoviack [Phys. Rev. B (2007)] finds that the phase behavior of the s+p spin-glass model is different from what proposed by Crisanti and Leuzzi [Phys. Rev. B 73, 014412 (2006)] if s and p are larger than two and are separated well enough. He proposes a trial picture, based on a one step replica symmetry breaking solution, displaying a mode-coupling-like glass-to-glass transition line ending in a A3 singularity. However, actually, the physics of these systems changes when p-s is large, the instability of which the one step replica symmetry breaking glassy phase suffers turns o…
We reply to the Comment by Hartmann (cond-mat/9908132) on our paper Phys. Rev. Lett. 84 (2000) 2026 (also cond-mat/9907125).
This is a reply to the comments by Richter and Chamberlin, and Diezemann and Bohmer to our paper (Phys. Rev. Lett. 85, 3448 (2000)). As further evidence for the claims in this Letter, we here reproduce the nonlinear spectral hole-burning experimental protocol in an equilibrated fully connected spin-glass model and we exhibit frequency selectivity, together with a shift in the base of the spectral hole.
In his Comment, Temesvári objects to a remark in our paper [Phys.\ Rev.\ B {\bf 91}, 104432 (2015)] that his result for the form of the Almeida-Thouless (AT) line obtained in an earlier paper with Parisi [Nucl.\ Phys.\ B {\bf 858}, 293 (2012)] in six dimensions can be obtained by taking the limit of $d \to 6$ in the equations valid for $d>6$, but that this violated one of the inequalities needed for their validity. He is just pointing out that they gave a derivation of the form of the AT line in six dimensions in [Nucl.\ Phys.\ B {\bf 858}, 293 (2012)] which avoided this difficulty. However, i…
Reply to Comment by Flenner and Szamel on our paper in Nature Physics 8, 164 (2012).
G. Brambilla et al. Reply to a Comment by J. Reinhardt et al. questioning the existence of equilibrium dynamics above the critical volume fraction of colloidal hard spheres predicted by mode coupling theory.
We review the phenomena of dynamical heterogeneity in glass-forming systems and its description within replica and mean-field theories of the glass transition.
We compare dynamical heterogeneities in equilibrated supercooled liquids and in the nonequilibrium glassy state within the framework of the random first order transition theory. Fluctuating mobility generation and transport in the glass are treated by numerically solving stochastic continuum equations for mobility and fictive temperature fields that arise from an extended mode coupling theory containing activated events. Fluctuating spatiotemporal structures in aging and rejuvenating glasses lead to dynamical heterogeneity in glasses with characteristics distinct from those found in the equili…
In their comment, Angelini et al. object to the conclusion of [J. Phys. A: Math. Theor., 52:445002, 2019] (1), where we show that in [Phys. Rev. B, 87:134201, 2013] the exponent $ν$ has been obtained by applying a mathematical relation in a regime where this relation is not valid. We observe that the criticism above on the mathematical validity of such relation has not been addressed in the comment. Our criticism thus remains valid, and disproves the conclusions of the comment. This constitutes the main point of this reply. We also provide a point-by-point response and discussion of Angelini e…
The existence of a generalized fluctuation-dissipation theorem observed in simulations and experiments performed in various glassy materials is related to the concepts of local equilibration and heterogeneity in space. Assuming the existence of a dynamic coherence length scale up to which the system is locally equilibrated, we extend previous generalizations of the FDT relating static to dynamic quantities to the physically relevant domain where asymptotic limits of large times and sizes are not reached. The formulation relies on a simple scaling argument and has thus not the character of a th…
We present simulation results suggesting that the stripe glass state described by Schmalian et al. for the Brazovskii model, cond-mat/0305420, may be dynamically unstable below the fluctuation-induced first-order transition temperature.
We study the growing time scales and length scales associated with dynamical slow down for a realistic glass former, using computer simulations. We perform finite size scaling to evaluate a length scale associated with dynamical heterogeneity which grows as temperature decreases. However, relaxation times which also grow with decreasing temperature, do not show the same kind of scaling behavior with system size as the dynamical heterogeneity, indicating that relaxation times are not solely determined by the length scale of dynamical heterogeneity. We show that relaxation times are instead dete…
Elasticity, Facilitation and Dynamic Heterogeneity in Glass-Forming liquids
本文通过二维粗粒化模型研究弹性诱导的促进对玻璃形成液体动力学的作用，发现其能重现动态非均匀性并解释玻璃化转变处动力学关联的涌现机制。
We examine the relation between the free volume per particle and the variance of the particle position, equivalent to a local Debye-Waller (DW) factor for a 2D glass-forming alloy using molecular dynamics simulations. We find that the latter quantity exhibits significant spatial heterogeneity despite involving trajectories two orders of magnitude shorter than those typically used to measure such heterogeneities. We find that the free volume exhibits no significant spatial correlation with the local DW factor. We conclude that the spatial variation in local free volume is not the cause of the s…
We propose and numerically implement a local probe of the static self-induced heterogeneity characterizing glass-forming liquids. The method relies on the equilibrium statistics of the overlap between pairs of configurations measured in mesoscopic cavities with unconstrained boundaries. By systematically changing the location of the probed cavity, we directly detect spatial variations of the overlap fluctuations. We provide a detailed analysis of the statistics of a local estimate of the configurational entropy and we infer an estimate of the surface tension between amorphous states, ingredien…
We conduct a numerical study of the dynamical behavior of a system of three-dimensional crosses, particles that consist of three mutually perpendicular line segments rigidly joined at their midpoints. In an earlier study [W. van Ketel et al., Phys. Rev. Lett. 94, 135703 (2005)] we showed that this model has the structural properties of an ideal gas, yet the dynamical properties of a strong glass former. In the present paper we report an extensive study of the dynamical heterogeneities that appear in this system in the regime where glassy behavior sets in. On the one hand, we find that the prop…
In this paper the phenomenon of dynamic heterogeneity in supercooled liquid systems is considered in terms of the recently proposed gauge theory of glass transition. The physical interpretation of the dynamic scaling is considered. It is shown that the development of the dynamic heterogeneity occurs due to the growth areas in which molecular motion is correlated due to the elastic interaction described by the gauge field. We obtains the analytical expressions for the dependence of the number of dynamically correlated atoms as the function on the system relaxation time, and the time dependence …
In this paper we consider in detail the properties of dynamical heterogeneity in lattice glass models (LGMs). LGMs are lattice models whose dynamical rules are based on thermodynamic, as opposed to purely kinetic, considerations. We devise a LGM that is not prone to crystallization and displays properties of a fragile glass-forming liquid. Particle motion in this model tends to be locally anisotropic on intermediate time scales even though the rules governing the model are isotropic. The model demonstrates violations of the Stokes-Einstein relation and the growth of various length scales assoc…
We construct the equations for the growth kinetics of an aging structural glass within mode-coupling theory through a non-stationary variant of the 3-density correlator defined in Phys. Rev. Lett. {\bf 97}, 195701 (2006). We solve a schematic form of the resulting equations to obtain the coarsening of the dynamic heterogeneity, characterized via the 3-point correlator $χ_3(t,t_w)$, as a function of waiting time $t_w$. For a quench into the glass, we find that $χ_3$ attains a peak value $\sim t_w^{0.5}$ at $t -t_w \sim t_w^{0.8}$, providing a theoretical basis for the numerical observations of …
In a recent letter, Kawasaki et al. (PRL 99, 215701 (2007)) study glass formation in a 2-dimensional (2D) model of polydisperse repulsive disks. They give numerical evidence for a direct relation between slowing down of the relaxation, extension of some medium-range order, and development of dynamic heterogeneities. We disagree with the authors' interpretation on two points which we believe to be potentially important for understanding the glass transition.
Dynamical heterogeneities -- strong fluctuations near the glass transition -- are believed to be crucial to explain much of the glass transition phenomenology. One possible hypothesis for their origin is that they emerge from soft (Goldstone) modes associated with a broken continuous symmetry under time reparametrizations. To test this hypothesis, we use numerical simulation data from four glass-forming models to construct coarse grained observables that probe the dynamical heterogeneity, and decompose the fluctuations of these observables into two transverse components associated with the pos…
We investigate a binary Lennard-Jones mixture with molecular dynamics simulations. We consider first a system cooled linearly in time with the cooling rate gamma. By varying gamma over almost four decades we study the influence of the cooling rate on the glass transition and on the resulting glass. We find for all investigated quantities a cooling rate dependence; with decreasing cooling rate the system falls out of equilibrium at decreasing temperatures, reaches lower enthalpies and obtains increasing local order. Next we study the dynamics of the melting process by investigating the most imm…
We test a hypothesis for the origin of dynamical heterogeneity in slowly relaxing systems, namely that it emerges from soft (Goldstone) modes associated with a broken continuous symmetry under time reparametrizations. We do this by constructing coarse grained observables and decomposing the fluctuations of these observables into transverse components, which are associated with the postulated time-fluctuation soft modes, and a longitudinal component, which represents the rest of the fluctuations. Our test is performed on data obtained in simulations of four models of structural glasses. As the …
We examined dynamic heterogeneity in a model tetrahedral network glass-forming liquid. We used four-point correlation functions to extract dynamic correlation lengths xi_4^a(t) and susceptibilities chi_4^a(t) corresponding to structural relaxation on two length scales a. One length scale corresponds to structural relaxation at nearest neighbor distances and the other corresponds to relaxation of the tetrahedral structure. We find that the dynamic correlation length xi_4^{a} grows much slower with increasing relaxation time than for model fragile glass formers. We also find that chi_4^a ~ (xi_4…
The dynamical heterogeneity in supercooled liquids measured by a molecular dynamics simulation has been quantified on the basis of the multifractal formalism. The singularity spectrum becomes broader as the glass transition is approached. This behavior is similar to that observed in the case of the Anderson-localization transition.
Dynamical heterogeneity and large deviations in the open quantum East glass model from tensor networks
利用张量网络方法研究耗散量子East模型的非平衡动力学，揭示了动力学异质性伴随慢弛豫，并发现了活性-非活性动力学相变的一阶特征。
We use the ``isoconfigurational ensemble'' [Phys. Rev. Lett. {\bf 93}, 135701 (2004)] to analyze both dynamical and structural properties in simulations of a glass forming molecular liquid. We show that spatially correlated clusters of low potential energy molecules are observable on the time scale of structural relaxation, despite the absence of spatial correlations of potential energy in the instantaneous structure of the system. We find that these structural heterogeneities correlate with dynamical heterogeneities in the form of clusters of low molecular mobility.
In Phys. Rev. Lett. 96, 035702 (2006) we introduced a class of kinetically constrained models which display a dynamical glass transition. We focused on a particular example: the "knights" model. As correctly pointed out by Jeng and Schwarz cond-mat/0612484, we overlooked some additional directed frozen structures of the knights model which are not simple directed percolation (DP) paths: these "thicker" directed structures lower the critical density. Here we argue that, nevertheless, the full directed processes are in the DP universality class and the T-junctions between perpendicular segments …
We study the relation between short-time vibrational modes and long-time relaxational dynamics in a kinetically constrained lattice gas with harmonic interactions between neighbouring particles. We find a correlation between the location of the low (high) frequency vibrational modes and regions of high (low) propensity for motion. This is similar to what was observed in continuous force systems, but our interpretation is different: in our case relaxation is due to localised excitations which propagate through the system; these localised excitations act as background disorder for the elastic ne…
Scaling Description of the Relaxation Dynamics and Dynamical Heterogeneity of an Active Glass-forming Liquid
本文通过分子动力学模拟和统一标度理论，研究了活性玻璃形成液体中活性涨落与密度涨落的耦合，揭示了活性增强密度涨落并导致从超阿伦尼乌斯到亚阿伦尼乌斯弛豫行为的动力学交叉，以及大活性下弛豫时间的非平凡系统尺寸依赖性。
Dynamical heterogeneity in active glasses is inherently different from its equilibrium behavior
该研究通过大规模模拟和解析模式耦合理论，发现活性玻璃的动力学异质性与其平衡行为本质不同，质疑了DH在玻璃态动力学中的核心作用。
Scaling Description of Dynamical Heterogeneity and Avalanches of Relaxation in Glass-Forming Liquids
本文提出玻璃形成液体中动力学异质性的标度理论，将动力学关联增长与零温固定点及雪崩型弛豫联系起来，并解释了 Stokes-Einstein 违背，预测得到弹塑性模型模拟验证。
The existence of heterogeneity in the dynamics of supercooled liquids is believed to be one of the hallmarks of the glass transition. Intense research has been carried out in the past to understand the origin of this heterogeneity in dynamics and a possible length scale associated with it. We have done extensive molecular dynamics simulations of few model glass-forming liquids in three dimensions to understand the temporal evolution of the dynamic heterogeneity and the heterogeneity length scale. We find that although the strength of the dynamic heterogeneity is maximum at a timescale close to…
We study dynamical heterogeneity and growing dynamical lengthscales in two kinetically constrained models, namely, the one- and two-vacancy assisted triangular lattice gases. One of the models is a strong glassformer and the other is a fragile glassformer. Both exhibit heterogeneous dynamics with broadly distributed timescales as seen in the distribution of persistence times. We show that the Stokes-Einstein relation is violated, to a greater degree in the fragile glassformer, and show how this violation is related to dynamic heterogeneity. We extract dynamical lengthscales from structure fact…
Glasses behave as solids due to their long relaxation time; however the origin of this slow response remains a puzzle. Growing dynamic length scales due to cooperative motion of particles are believed to be central to the understanding of both the slow dynamics and the emergence of rigidity. Here, we provide experimental evidence of a growing dynamical heterogeneity length scale that increases with increasing waiting time in an aging colloidal glass of Laponite. The signature of heterogeneity in the dynamics follows from dynamic light scattering measurements in which we study both the rotation…
Different glassy characteristics are related to either caging or dynamical heterogeneity
本研究通过解析论证与多维度系统模拟，揭示玻璃态特征源于颗粒禁禁闭与动力学异质性两种机制，为玻璃态动力学数据分析及理论构建提供了严格约束。
Using molecular dynamics simulations, we have determined that the nature of dynamical heterogeneity in jammed liquids is very sensitive to short-ranged attractions. Weakly attractive systems differ little from dense hard-sphere and Lennard-Jones fluids: Particle motion is punctuated and tends to proceed in steps of roughly a single particle diameter. Both of these basic features change in the presence of appreciable attractions. Transient periods of particle mobility and immobility cannot be discerned at intermediate attraction strength, for which structural relaxation is greatly enhanced. Str…
We investigate the growth of dynamic heterogeneity in a glassy hard-sphere mixture for volume fractions up to and including the mode-coupling transition. We use an 80 000 particle system to test a new procedure to evaluate a dynamic correlation length xi(t): we determine the ensemble independent dynamic susceptibility chi_4(t) and use it to facilitate evaluation of xi(t) from the small wave vector behavior of the four-point structure factor. We analyze relations between the alpha relaxation time tau_alpha, chi_4(tau_alpha), and xi(tau_alpha). We find that mode-coupling like power laws provide …
As liquids approach the glass transition temperature, dynamical heterogeneity emerges as a crucial universal feature of their behavior. Dynamic facilitation, where local motion triggers further motion nearby, plays a major role in this phenomenon. Here we show that long-range, elastically-mediated facilitation appears below the mode-coupling temperature, adding to the short-range component present at all temperatures. Our results suggest deep connections between the supercooled liquid and glass states, and pave the way for a deeper understanding of dynamical heterogeneity in glassy systems.
Reply to "Comment on 'Fickian non-Gaussian diffusion in glass-forming liquids' ". In [ArXiv:2210.07119v1], Berthier et al. questioned the findings of our letter [Phys. Rev. Lett. 128, 168001 (2022)], concerning the existence and the features of Fickian non-Gaussian diffusion in glass-forming liquids. Here we demonstrate that their arguments are either wrong, or not meaningful to our scope. Thus, we fully confirm the validity and novelty of our results.
The effects of randomly pinning particles in a model glass-forming fluid are studied, with a focus on the dynamically heterogeneous relaxation in the presence of pinning. We show how four-point dynamical correlations can be analysed in real space, allowing direct extraction of a length scale that characterises dynamical heterogeneity. In the presence of pinning, the relaxation time of the glassy system increases by up to two decades, but there is almost no increase in either the four-point correlation length or the strength of the four-point correlations. We discuss the implications of these r…
The dynamics of a bilayer system of ultracold dipolar molecules exhibits classical and quantum glassy behavior, characterized by long tails in the relaxation time and dynamical heterogeneity. In the proposed setup, quantum fluctuations are of the order of thermal fluctuations and the degree of frustration can tuned by the interlayer distance. We present experimental accessible order parameters based on marker molecules, distinguished by properly chosen internal levels, and find quantum features of dynamical heterogeneity.
Kinetically constrained spin models are schematic coarse-grained models for the glass transition which represent an efficient theoretical tool to study detailed spatio-temporal aspects of dynamic heterogeneity in supercooled liquids. Here, we study how spatially correlated dynamic domains evolve with time and compare our results to various experimental and numerical investigations. We find that strong and fragile models yield different results. In particular, the lifetime of dynamic heterogeneity remains constant and roughly equal to the alpha relaxation time in strong models, while it increas…
Recent work has demonstrated the strong qualitative differences between the dynamics near a glass transition driven by short-ranged repulsion and one governed by short-ranged attraction. Here, we study in detail the behavior of non-linear, higher-order correlation functions that measure the growth of length scales associated with dynamical heterogeneity in both types of systems. We find that this measure is qualitatively different in the repulsive and attractive cases with regards to the wave vector dependence as well as the time dependence of the standard non-linear four-point dynamical susce…
We consider the problem of slow activation dynamics in glassy systems undergoing a random first order phase transition. Using an effective potential approach to supercooled liquids, we determine the spectrum of activation barriers for entropic droplets. We demonstrate that fluctuations of the configurational entropy and of the liquid glass surface tension are crucial to achieve an understanding of the barrier fluctuations in glassy systems and thus are ultimatively responsible for the broad spectrum of excitations and heterogeneous dynamics in glasses. In particular we derive a relation betwee…
Polydispersity is found to have a significant effect on the potential energy landscape; the the average inherent structure energy with temperature decreases with polydispersity. Increasing polydispersity at fixed volume fraction decreases the glass transition temperature and the fragility of glass formation analogous to the antiplasticization seen in some polymeric melts. An interesting temperature dependent crossover of heterogeneity with polydispersity is observed at low temperature due to the faster build-up of dynamic heterogeneity at lower polydispersity.
Dynamic heterogeneity in glass-formers has been related to their static structure using the concept of dynamic propensity. We re-examine this relationship by analyzing dynamical fluctuations in two atomistic glass-formers and two theoretical models. We introduce quantitative statistical indicators which show that the dynamics of individual particles cannot be predicted on the basis of the propensity, nor by any structural indicator. However, the spatial structure of the propensity field does have predictive power for the spatial correlations associated with dynamic heterogeneity. Our results s…
We examine the phenomenon of dynamical heterogeneity in computer simulations of an equilibrium, glass-forming liquid. We describe several approaches to quantify the spatial correlation of single-particle motion, and show that spatial correlations of particle displacements become increasingly long-range as the temperature decreases toward the mode coupling critical temperature.
We consider the probability distribution for fluctuations in dynamical action and similar quantities related to dynamic heterogeneity. We argue that the so-called "glass transition" is a manifestation of low action tails in these distributions where the entropy of trajectory space is sub-extensive in time. These low action tails are a consequence of dynamic heterogeneity and an indication of phase coexistence in trajectory space. The glass transition, where the system falls out of equilibrium, is then an order-disorder phenomenon in space-time occurring at a temperature T_g which is a weak fun…
The routine transformation of a liquid, as it is cooled rapidly, resulting in glass formation, is remarkably complex. A theoretical explanation of the dynamics associated with this process has remained one of the major unsolved problems in condensed matter physics. The Random First Order Transition (RFOT) theory, which was proposed over twenty five years ago, provides a theoretical basis for explaining much of the phenomena associated with glass forming materials. It links or relates multiple metastable states, slow or glassy dynamics, dynamic heterogeneity, and both a dynamical and an ideal g…
Dynamic heterogeneity is now recognised as a central aspect of structural relaxation in disordered materials with slow dynamics, and was the focus of intense research in the last decade. Here we describe how initial, indirect observations of dynamic heterogeneity have recently evolved into well-defined, quantitative, statistical characterisations, in particular through the use of high-order correlation and response functions. We highlight both recent progress and open questions about the characterisation of dynamic heterogeneity in glassy materials. We also discuss the limits of available tool…
Macroscopic active matter under confinement: dynamical heterogeneity, bursts, and glassy behavior in a few-body system of self-propelling camphor surfers
研究自推进山梨糖浆游动体在圆形边界内的集体动力学，揭示密度依赖的爆发现象和玻璃行为。
Amorphous solids are mechanically rigid while possessing a disordered structure similar to that of dense liquids. Recent research indicates that dynamical heterogeneity, spatio-temporal fluctuations in local dynamical behavior, might help understanding the statistical mechanics of glassy states.
Non-Gaussian nature of the probability distribution of particles' displacements in the supercooled temperature regime in glass-forming liquids are believed to be one of the major hallmarks of glass transition. It is already been established that this probability distribution which is also known as the van Hove function show universal exponential tail. The origin of such an exponential tail in the distribution function is attributed to the hopping motion of particles observed in the supercooled regime. The non-Gaussian nature can also be explained if one assumes that the system has heterogeneou…
In a recent paper [P. Mayer et al., Phys. Rev. Lett. 93, 115701 (2004)] it was shown, by means of experiments, theory and simulations, that coarsening systems display dynamic heterogeneity analogous to that of glass formers. Here, we present a detailed analysis of dynamic heterogeneities in the Glauber-Ising chain. We discuss how dynamic heterogeneity in Ising systems must be measured through connected multi-point correlation functions. We show that in the coarsening regime of the Ising chain these multi-point functions reveal the growth of spatial correlations in the dynamics, beyond what can…
Probing dynamic and static correlation in glass-forming supercooled liquids has been a challenge for decades in spite of extensive research. Dynamic correlation which manifests itself as Dynamic Heterogeneity is ubiquitous in a vast variety of systems starting from molecular glass-forming liquids, dense colloidal systems to collections of cells. On the other hand, the mere concept of static correlation in these dense disordered systems remain somewhat elusive and its existence is still actively debated. We propose a novel method to extract both dynamic and static correlations using rod-like pa…
We study glass behavior in a mixture of elliptic and circular particles in two dimensions at low temperatures using an orientation-dependent Lennard-Jones potential. The ellipses have a mild aspect ratio ($\sim 1.2$) and tend to align at low temperatures, while the circular particles play the role of impurities disturbing the ellipse orientations at a concentration of 20%. These impurities have a size smaller than that of the ellipses and attract them in the homeotropic alignment. As a result, the coordination number around each impurity is mostly five or four in glassy states. We realize doub…
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