We report nano-scale mechanical heterogeneity of a metallic glass characterized by dynamic atomic force microscopy. Apparent energy dissipation with the variation of ~12%, originating from non-uniform distribution of local viscoelasticity, was characterized. The correlation length of heterogeneous viscoelasticity was measured to be ~2.5{\pm}0.3 nm, which is well consistent with the dimension of shear transformation zones for plastic flow. This study provides the first experimental observation on the nano-scale mechanical heterogeneity in a metallic glass, and may fill the gap between atomic models and the macroscopic properties of metallic glasses.
We have carried out time--domain electrostatic force spectroscopy on two different ion conducting glasses using an atomic force microscope. We compare the electrostatic force spectroscopic data obtained at different temperatures with macroscopic electrical data of the glasses. The overall consistency of the data shows that electrostatic force spectroscopy is capable of probing the ion dynamics and transport in nanoscopic subvolumes of the samples.
We show the correlation between nanoscale structural heterogeneity and mechanical property and glass forming ability of Zr-based metallic glasses (MGs). Detailed parameters of medium range ordering (MRO) that constitutes the structural heterogeneity, including the type, size, and volume fraction of MRO domains determined using 4-dimensional scanning transmission electron microscopy, directly correlate with the ductility and glass forming ability of Zr-Cu-Co-Al MGs. Mesoscale deformation simulation incorporating the experimentally determined MRO confirms that the diverse types and sizes of MRO …
The existence of nanoscale ductility during the fracture of silicate glasses remains controversial. Here, based on molecular dynamics simulations coupled with topological constraint theory, we show that nano-ductility arises from the spatial heterogeneity of the atomic network's rigidity. Specifically, we report that localized floppy modes of deformation in under-constrained regions of the glass enable plastic deformations of the network, resulting in permanent change in bond configurations. Ultimately, these heterogeneous plastic events percolate, thereby resulting in a non-brittle mode of fr…
Cryogenic rejuvenation in metallic glasses reported in Ketov et al 's experiment (Nature(2015)524,200) has attracted much attention, both in experiments and numerical studies. The atomic mechanism of rejuvenation has been conjectured to be related to the heterogeneity of the glassy state, but the quantitative evidence is still elusive. Here we use molecular dynamics simulations of a model metallic glass to investigate the heterogeneity in the local thermal expansion. We then combine the resulting spatial distribution of thermal expansion with a continuum mechanics calculation to infer the inte…
We report results of molecular dynamics simulations of a binary Lennard-Jones system at zero pressure in the undercooled liquid and glassy states. We first follow the evolution of diffusivity and dynamic heterogeneity with temperature and show their correlation. In a second step we follow the ageing of a quenched glass. As diffusivity decreases with ageing, heterogeneity increases. We conclude that the heterogeneity is a property of the inherent diffusion of the relaxed state. The variations with aging time can be explained by annealing of quenched defect structures. This annealing has the sam…
We review the phenomena of dynamical heterogeneity in glass-forming systems and its description within replica and mean-field theories of the glass transition.
Using atomistic computer simulations we determine the roughness and topographical features of melt-formed (MS) and fracture surfaces (FS) of oxide glasses. We find that the topography of the MS is described well by the frozen capillary wave theory. The FS are significant rougher than the MS and depend strongly on glass composition. The height-height correlation function for the FS shows an unexpected logarithmic dependence on distance, in contrast to the power-law found in experiments. We thus conclude that on length scales less than 10 nm FS are not self-affine fractals.
Dynamic heterogeneity as one of the most important properties in supercooled liquids has been found for several decades. However, its structural origin remains open for many systems. Here, we propose a new structural parameter to characterize local atomic packing in metallic liquids. It is found that the new parameter in a simulated metallic glass-forming liquid is closely correlated with potential energy and atomic mobility. It also exhibits significant spatial heterogeneities and these structural fluctuations show close correlation with the spatial distribution of the long-time dynamic prope…
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)].
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 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…
The most puzzling aspect of the glass transition observed in laboratory is an apparent decoupling of dynamics from structure. In this paper we recount the implication of various theories of glass transition for the static correlation length in an attempt to reconcile the dynamic and static lengths associate with the glass problem. We argue that a more recent characterization of the static relaxation length based on the bond ordering scenario, as the typical length over which the energy fluctuations are correlated, is more consistent with, and indeed in perfect agreement with the typical linear…
Response functions and fluctuations measured locally in complex materials should equally well characterize mesoscopic-scale dynamics. The fluctuation-dissipation-relation (FDR), relates the two in equilibrium, a fact used regularly, for example, to infer mechanical properties of soft matter from the fluctuations in light scattering. In slowly-evolving non-equilibrium systems, such as aging spin and structural glasses, sheared soft matter, and active matter, a form of FDR has been proposed in which an effective temperature, Teff, replaces the usual temperature, and universal behavior is found i…
We demonstrate through two case studies, one on the p-spin interaction model and the other on the random K-satisfiability problem, that a heterogeneity transition occurs to the ground-state configuration space of a random finite-connectivity spin glass system at certain critical value of the constraint density. At the transition point, exponentially many configuration communities emerge from the ground-state configuration space, making the entropy density s(q) of configuration-pairs a non-concave function of configuration-pair overlap q. Each configuration community is a collection of relative…
We report an investigation of the heterogeneity in super-cooled liquids and glasses using the non-Gaussianity parameter. We simulate selenium and a binary Lennard-Jones system by molecular dynamics. In the non-Gaussianity three time domains can be distinguished. First there is an increase on the ps-scale due to the vibrational (ballistic) motion of the atoms. This is followed, on an intermediate time-scale, by a growth, due to local relaxations (beta-relaxation) at not too high temperatures. A maximum is reached at times corresponding to long range diffusion (alpha-relaxation). At long times t…
Rayleigh anomalies and disorder-induced mixing of polarizations at nanoscale in amorphous solids. Testing 1-octyl-3-methylimidazolium chloride glass
Universitá degli studi di Roma ”La Sapienza”（罗马第一大学）；Istituto Italiano di Tecnologia - Center for Life Nanoscience（意大利理工大学-生命纳米科学中心）；University of Geneva（日内瓦大学）；Chalmers University of Technology（查尔姆斯理工大学）；Sincrotrone Trieste S.C.p.A.（的里雅斯特同步辐射中心）
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 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 …
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…
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 study the local dynamical fluctuations in glass-forming models of particles embedded in $d$-dimensional space, in the mean-field limit of $d\to\infty$. Our analytical calculation reveals that single-particle observables, such as squared particle displacements, display divergent fluctuations around the dynamical (or mode-coupling) transition, due to the emergence of nontrivial correlations between displacements along different directions. This effect notably gives rise to a divergent non-Gaussian parameter, $α_2$. The $d\to\infty$ local dynamics therefore becomes quite rich upon approaching …
Recent experiments and computer simulations show that supercooled liquids around the glass transition temperature are "dynamically heterogeneous" [1]. Such heterogeneity is expected from the random first order transition theory of the glass transition. Using a microscopic approach based on this theory, we derive a relation between the departure from Debye relaxation as characterized by the $β$ value of a stretched exponential response function $ϕ(t) =e^{-(t/ τ_{KWW})^β}$, and the fragility of the liquid. The $β$ value is also predicted to depend on temperature and to vanish as the ideal glass …
The relationship between spatially heterogeneous dynamics (SHD) and jamming is studied in a glass-forming binary Lennard-Jones system via molecular dynamics simulations. It has been suggested that the probability distribution of interparticle forces $P(F)$ develops a peak at the glass transition temperature $T_g$, and that the large force inhomogeneities, responsible for structural arrest in granular materials, are related to dynamical heterogeneities in supercooled liquids that form glasses. It has been further suggested that ``force chains'' present in granular materials may exist in superco…
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…
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 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 …
The glassy dynamics of plastic-crystalline cyclo-octanol and ortho-carborane, where only the molecular reorientational degrees of freedom freeze without long-range order, is investigated by nonlinear dielectric spectroscopy. Marked differences to canonical glass formers show up: While molecular cooperativity governs the glassy freezing, it leads to a much weaker slowing down of molecular dynamics than in supercooled liquids. Moreover, the observed nonlinear effects cannot be explained with the same heterogeneity scenario recently applied to canonical glass formers. This supports ideas that mol…
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…
Dynamical heterogeneity and large deviations in the open quantum East glass model from tensor networks
University of Nottingham（诺丁汉大学）；Centre for the Mathematics and Theoretical Physics of Quantum Non-Equilibrium Systems, University of Nottingham（诺丁汉大学量子非平衡系统数学与理论物理中心）；Max-Planck-Institut für Quantenoptik（马克斯·普朗克量子光学研究所）；Munich Center for Quantum Science and Technology (MCQST)（慕尼黑量子科学与技术中心）
Polarization fluctuations were measured in nanoscale volumes of a polymer glass during aging following a temperature quench through the glass transition. Statistical properties of the noise were studied in equilibrium and during aging. The noise spectral density had a larger temporal variance during aging, i.e. the noise was more non-Gaussian, demonstrating stronger correlations during aging.
Cycling of a metallic glass between ambient and cryogenic temperatures can induce higher-energy states characteristic of glass formation on faster cooling. This rejuvenation, unexpected because it occurs at small macroscopic strains and well below the temperatures of thermally induced structural change, is important, for example, in improving plasticity. Molecular-dynamics simulations elucidate the mechanisms by which thermal cycling can induce relaxation (reaching lower energy) as well as rejuvenation. Thermal cycling, over tens of cycles, drives local atomic rearrangements progressively eras…
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…
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.
Glass-forming liquids grow dramatically sluggish upon cooling. This slowdown has long been thought to be accompanied by a growing correlation length. Characteristic dynamical and static length scales, however, have been observed to grow at different rates, which perplexes the relationship between the two and with the slowdown. Here, we show the existence of a direct link between dynamical sluggishness and static point-to-set correlations, holding at the local level as we probe different environments within a liquid. This link, which is stronger and more general than that observed with locally …
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.
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…
We propose a spatio-temporal characterization of the entanglement dynamics in many-body localized (MBL) systems, which exhibits a striking resemblance with dynamical heterogeneity in classical glasses. Specifically, we find that the relaxation times of local entanglement, as measured by the concurrence, are spatially correlated yielding a dynamical length scale for quantum entanglement. As a consequence of this spatio-temporal analysis, we observe that the considered MBL system is made up of dynamically correlated clusters with a size set by this entanglement length scale. The system decompose…
A theoretical treatment of deeply supercooled liquids is difficult because their properties emerge from spatial inhomogeneities that are self-induced, transient, and nanoscopic. I use computer simulations to analyse self-induced static and dynamic heterogeneity in equilibrium systems approaching the experimental glass transition. I characterise the broad sample-to-sample fluctuations of salient dynamic and thermodynamic properties in elementary mesoscopic systems. Findings regarding local lifetimes and distributions of dynamic heterogeneity are in excellent agreement with recent single molecul…
We use molecular dynamic simulations to investigate the relation between the presence of packing defects in a glass-former and the spontaneous cooperative motions called dynamic heterogeneity. For that purpose we use a simple diatomic glass-former and add a small number of larger or smaller diatomic probes. The diluted probes modify locally the packing, inducing structural defects in the liquid, while we find that the number of defects is small enough not to disturb the average structure. We find that a small packing modification around a few molecules can deeply influence the dynamics of the …
