Dynamics Of Metallic Glass Research Articles

Coupling structural, chemical composition and stress fluctuations with relaxation dynamics in metallic glasses

Understanding the atomistic mechanisms of relaxation dynamics in metallic glasses remains a longstanding challenge. Here, using microsecond time scale molecular dynamics simulations, three main relaxation stages in metallic glasses are identified. At about 0.6Tg, chemical composition plays a dominant role in the relaxation, manifested by stress accumulation and only minimal variations in structure. As Tg approaches, the confluence of structural heterogeneity and chemical composition leads to the decoupling of relaxation mechanisms. At this temperature, the relaxation results in a structure with a lower energy state and a lower level of stress. In the supercooled liquid regime, an extensive increase in the number of closed-packed icosahedral clusters is responsible for accelerated structural relaxation while their packing frustration leads to the accumulation of intrinsic residual stresses in the glass. The atomistic origin of these dynamic relaxation modes is discussed in terms of structural, chemical composition and stress variations.

Strain-dependent transition of the relaxation dynamics in metallic glasses

Non-exponential relaxation is pervasive in glassy systems and intimately related to unique thermodynamic features, such as glass transition and aging; however, the underlying mechanisms remain unclear. The time scale of non-exponential relaxation goes beyond the time limit (nanosecond) of classic molecular dynamics simulation. Thus, the advanced time scaling atomistic approach is necessary to interpret the relaxation mechanisms at the experimental timescale. Here, we adopted autonomous basin climbing (ABC) to evaluate the long-time stress relaxation. At the same time, based on the energy minimization principle, we carried out simulations at continuum levels on the long-time stress relaxation kinetics of Cu–Zr metallic glass over timescales greater than 100 s. Combined with atomistic and continuum models, we demonstrate that a strain-dependent transition from compressed to stretched exponentials would happen, consistent with recent experimental observations on metallic glasses. Further examination of the spatial and temporal correlations of stress and plastic strain reveals two predominant driving forces: the thermal energy gradient governs in the compressed regime and leads to a release of the local internal stress; in the stretched regime, the strain energy gradient rules and causes long-range structural rearrangements. The discovery of the competition between two driving forces advances our understanding of the nature of aging dynamics in disordered solids.

Beam Effects on Atomic Dynamics in Metallic Glasses Studied With Electron Correlation Microscopy.

Electron correlation microscopy (ECM) is used to investigate atomic dynamics in metallic glasses (MG) close to metastable equilibrium. It temporally correlates diffracted intensities of a time series of dark-field images to deduce a metric for structural decays. The measurement parameters, such as time and temperature, must be chosen according to the material of interest. In this work, ECM was extended to measurements at room temperature. To ensure, or select, a time window with quasi-thermodynamic equilibrium/steady-state measurement conditions, two-time correlation functions of diffracted intensities were calculated. The dynamics at room temperature are partly driven by the electron beam, thus affecting the material and the results. A systematic analysis of the influence of the electron beam is presented, revealing an inverse relation between electron dose rate and intensity correlation decay times at 300 kV acceleration voltage. However, the underlying dynamical mechanisms, described by a stretching exponent, are found to be independent of the applied electron dose rate for a Pd40Ni40P20 MG. An extrapolation of the results to infinite long measurement times and zero dose rate agrees with X-ray photon correlation spectroscopy data and justifies the application of beam-driven ECM at room temperature to study the dynamics of disordered systems.

Micro-scaled plastic yielding and shear-banding dynamics in metallic glasses

Shear-banding behavior in metallic glasses plays a key role in the operation of plastic deformation, which is associated with yield strength. In a micro-scale, the shear-banding behavior must be affected by many factors from the test machine and the substrate. Therefore, in this study, comprehensively considering a machine compliance, a geometry imperfection of micro-pillar, and a substrate sink- in the machine-sample-substrate system, we developed a plastic-strength model at a micrometer scale in this study, which is evidenced by the microscale compressive properties of 18 kinds of metallic glasses. The theoretical model provides a guidance for the elastic limits and shear-banding dynamics of metallic glasses at the micro-scale, which can be applicable to characterize the microscale deformation behavior of other amorphous materials.

Indentation creep dynamics in metallic glasses under different structural states

In this study, the effects of the structural energy states (as-cast and relaxed) of Zr50Cu40Al10 metallic glass were investigated using depth-sensing nanoindentation. In terms of cooperative shear model, we performed experimental characterization of shear transformation zone for plastic flow of metallic glass. The shear transformation zone volume of the relaxed metallic glass is larger than that of as-cast one, while the strain rates sensitivity displays the opposite tendency. The plastic deformation in the creep stage of nanoindentation originates from the “delayed plasticity” inherited from the loading process. The creep depth shows strain rates and microstructural states dependence. The characteristic relaxation time and creep depth limit were determined by fitting the displacement versus time curves with Kelvin model are employed to characterize the creep dynamics of metallic glasses. It was found that the softening effects in the plastic deformation originates from the collective movements of the deformation carriers (shear transformation zones). The different softening behaviors were discussed from the perspective of soft zones in the framework of the free volume model. Our experimental as well as the theoretical analysis deepens the fundamental understanding of plasticity deformation mechanism in metallic glasses.

Vitrification decoupling from α-relaxation in a metallic glass.

Understanding how glasses form, the so-called vitrification, remains a major challenge in materials science. Here, we study vitrification kinetics, in terms of the limiting fictive temperature, and atomic mobility related to the α-relaxation of an Au-based bulk metallic glass former by fast scanning calorimetry. We show that the time scale of the α-relaxation exhibits super-Arrhenius temperature dependence typical of fragile liquids. In contrast, vitrification kinetics displays milder temperature dependence at moderate undercooling, and thereby, vitrification takes place at temperatures lower than those associated to the α-relaxation. This finding challenges the paradigmatic view based on a one-to-one correlation between vitrification, leading to the glass transition, and the α-relaxation. We provide arguments that at moderate to deep undercooling, other atomic motions, which are not involved in the α-relaxation and that originate from the heterogeneous dynamics in metallic glasses, contribute to vitrification. Implications from the viewpoint of glasses fundamental properties are discussed.

Thermal History Dependent Aging Dynamics in a La-Based Metallic Glass

The atomic dynamics in metallic glasses (MGs) are closely related to their stability. Due to weak resistance to nanocrystallization at high temperatures, we interestingly observe the slow atomic dynamics happening in an as-quenched La-Al-Ni MG sample compared with a sub-Tg pre-annealed one when cooling from about 0.99Tg (Tg the glass transition temperature). An intermittent aging behavior also appears in the as-quenched MG sample only on cooling but not on heating, nor does it appear in the pre-annealed sample on both cooling and heating, indicating that it could be thermal history dependent and related to the existence of nanocrystals. Differently, a sudden atomic dynamics transition from fast to slow is observed in the pre-annealed MG sample when the pre-annealing temperature is approached upon cooling, resulting from the configuration recovery to a low energy state created by pre-annealing. Our findings demonstrate that the thermal history can give rise to significantly different aging dynamics of MGs , providing an in-depth understanding of structural relaxation in disordered materials on the atomic level.

Plastic Dynamical Model for Bulk Metallic Glasses

Based on previous experimental results of the plastic dynamic analysis of metallic glasses upon compressive loading, a dynamical model is proposed. This model includes the sliding speed of shear bands in the plastically strained metallic glasses, the shear resistance of shear bands, the internal friction resulting from plastic deformation, and the influences from the testing machine. This model analysis quantitatively predicts that the loading rate can influence the transition of the plastic dynamics in metallic glasses from chaotic (low loading rate range) to stable behavior (high loading rate range), which is consistent with the previous experimental results on the compression tests of a Cu50Zr45Ti5 metallic glass. Moreover, we investigate the existence of a nonconstant periodic solution for plastic dynamical model of bulk metallic glasses by using Manásevich–Mawhin continuation theorem.

Static atomic-scale structural heterogeneity and its effects on glass formation and dynamics of metallic glasses

Molecular dynamics simulations were employed to investigate structural heterogeneity at the sub-nanometer scale for binary Cu-Zr liquids and glasses. The normalized local atomic number density fluctuates significantly in all the liquids and glasses, confirming existence of the static atomic-scale structural heterogeneity. The dynamic evolution of structural heterogeneity profile shows that the good glass former has better inheritance of structural heterogeneity from its liquid state than the poor one, suggesting a close relation between the structural inheritance and the glass-forming ability. Further analyses regarding evolution of dynamic properties, i.e., viscosity and the α relaxation time, as a function of undercooling demonstrate that the better inheritance of the structural heterogeneity in the better glass former stems from its higher liquid stability. Our atomic structural investigation indicates that the enhanced connectivity of short-range ordering clusters could be responsible for the better inheritance of structural heterogeneity and the larger glass-forming ability.

Local structural mechanism for frozen-in dynamics in metallic glasses

The nature of the glass transition is a fundamental and long-standing intriguing issue in the condensed-matter physics and materials science community. In particular, the structural response by which a liquid is arrested dynamically to form a glass or amorphous solid upon approaching its freezing temperature [the glass transition temperature (${T}_{g}$)] remains unclear. Various structural scenarios in terms of the percolation theory have been proposed recently to understand such a phenomenon; however, there is still no consensus on what the general percolation entity is and how the entity responds to the sudden slowdown dynamics during the glass transition. In this paper, we demonstrate that one-dimensional local linear ordering (LLO) is a universal structural motif associated with the glass transition for various metallic glasses. The quantitative evolution of LLO with temperature indicates that a percolating LLO network forms to serve as the backbone of the rigid glass solid when the temperature approaches the freezing point, resulting in the frozen-in dynamics accompanying the glass transition. The percolation transition occurs by pinning different LLO networks together, which only needs the introduction of a small number of ``joint'' atoms between them, and therefore the energy expenditure is very low.

Correlation between Local Structure Order and Spatial Heterogeneity in a Metallic Glass.

Although nanoscale spatial heterogeneity of metallic glasses has been demonstrated by extensive experimental and theoretical investigations, the nature of spatial heterogeneity remains poorly known owing to the absence of a structural depiction of the inhomogeneity from experimental insight. Here we report the experimental characterization of the spatial heterogeneity of a metallic glass by utilizing state-of-the-art angstrom-beam electron diffraction and scanning transmission electron microscopy. The subnanoscale electron diffraction reveals that the nanoscale spatial heterogeneity and corresponding density fluctuation have a close correlation with the local structure variation from icosahedronlike to tetragonal crystal-like order. The structural insights of spatial heterogeneity have important implications in understanding the properties and dynamics of metallic glasses.

Temperature dependence of the kinetic energy in the Zr40Be60 amorphous alloy

The average kinetic energy 〈E(T)〉 of the atomic nucleus for each element of the amorphous alloy Zr40Be60 in the temperature range 10–300 K has been measured for the first time using VESUVIO spectrometer (ISIS). The experimental values of 〈E(T)〉 have been compared to the partial ZrBe spectra refined by a recursion method based on the data obtained with thermal neutron scattering. The satisfactory agreement has been reached with the calculations using partial spectra based on thermal neutron spectra obtained with recursion method. In addition, the experimental data have been compared to the Debye model. The measurements at different temperatures (10, 200, and 300 K) will provide an opportunity to evaluate the significance of anharmonicity in the dynamics of metallic glasses.

A microscopic continuum model for defect dynamics in metallic glasses

Motivated by results of the topological theory of glasses accounting for geometric frustration, we develop the simplest possible continuum mechanical model of defect dynamics in metallic glasses that accounts for topological, energetic, and kinetic ideas. A geometrical description of ingredients of the structure of metallic glasses using the concept of local order based on Frank–Kasper phases and the notion of disclinations as topological defects in these structures is proposed. This novel kinematics is incorporated in a continuum mechanical framework capable of describing the interactions of disclinations and also of dislocations (interpreted as pairs of opposite disclinations). The model is aimed towards the development of a microscopic understanding of the plasticity of such materials. We discuss the expected predictive capabilities of the model vis-a-vis some observed physical behaviors of metallic glasses.

Universal slip dynamics in metallic glasses and granular matter \u2013 linking frictional weakening with inertial effects

Slowly strained solids deform via intermittent slips that exhibit a material-independent critical size distribution. Here, by comparing two disparate systems - granular materials and bulk metallic glasses - we show evidence that not only the statistics of slips but also their dynamics are remarkably similar, i.e. independent of the microscopic details of the material. By resolving and comparing the full time evolution of avalanches in bulk metallic glasses and granular materials, we uncover a regime of universal deformation dynamics. We experimentally verify the predicted universal scaling functions for the dynamics of individual avalanches in both systems, and show that both the slip statistics and dynamics are independent of the scale and details of the material structure and interactions, thus settling a long-standing debate as to whether or not the claim of universality includes only the slip statistics or also the slip dynamics. The results imply that the frictional weakening in granular materials and the interplay of damping, weakening and inertial effects in bulk metallic glasses have strikingly similar effects on the slip dynamics. These results are important for transferring experimental results across scales and material structures in a single theory of deformation dynamics.

Probing the evolution of slow flow dynamics in metallic glasses

The dynamics of glass is of paramount importance for understanding glass, while experimental studies of it covering broad time and temperature ranges are fraught with difficulty. We employ a method which can probe the extremely slow dynamics in various glassy states in metallic glass (MG). The flow dynamics of as-cast MG is found to follow a universal Arrhenius behavior in a wide temperature range, and aged MG follows a stretched exponential function with a ``magic'' exponent number of 3/7. Our observations have implications for understanding the structural evolution of the slow flow and the issue of finite temperature divergence in MGs.

Unveiling the structural arrangements responsible for the atomic dynamics in metallic glasses during physical aging.

Understanding and controlling physical aging, that is, the spontaneous temporal evolution of out-of-equilibrium systems, represents one of the greatest tasks in material science. Recent studies have revealed the existence of a complex atomic motion in metallic glasses, with different aging regimes in contrast with the typical continuous aging observed in macroscopic quantities. By combining dynamical and structural synchrotron techniques, here for the first time we directly connect previously identified microscopic structural mechanisms with the peculiar atomic motion, providing a broader unique view of their complexity. We show that the atomic scale is dominated by the interplay between two processes: rearrangements releasing residual stresses related to a cascade mechanism of relaxation, and medium range ordering processes, which do not affect the local density, likely due to localized relaxations of liquid-like regions. As temperature increases, a surprising additional secondary relaxation process sets in, together with a faster medium range ordering, likely precursors of crystallization.

Unusual fast secondary relaxation in metallic glass.

The relaxation spectrum of glassy solids has long been used to probe their dynamic structural features and the fundamental deformation mechanisms. Structurally complicated glasses, such as molecular glasses, often exhibit multiple relaxation processes. By comparison, metallic glasses have a simple atomic structure with dense atomic packing, and their relaxation spectra were commonly found to be simpler than those of molecular glasses. Here we show the compelling evidence obtained across a wide range of temperatures and frequencies from a La-based metallic glass, which clearly shows two peaks of secondary relaxations (fast versus slow) in addition to the primary relaxation peak. The discovery of the unusual fast secondary relaxation unveils the complicated relaxation dynamics in metallic glasses and, more importantly, provides us the clues which help decode the structural features serving as the ‘trigger' of inelasticity on mechanical agitations.

Shear‐Band Dynamics in Metallic Glasses

The future of metallic glasses as an advanced structural and functional material will to a great extent depend on the understanding and control of their mesoscopic flow defects called shear bands. These defects are sweet‐and‐sour; sweet because they mediate macroscopic plasticity at room temperature, and sour because they quickly promote failure. In the past decade, fundamental research generated great progress in characterizing the role that shear bands play during plastic deformation of disordered systems, including metallic glasses. Similar to those in many other materials, shear bands in metallic glasses are only active for a very short time, which directed research focus towards topological, structural, chemical, and thermal properties of formed, but inactive shear bands. In this paper, recent progress in directly characterizing the shear‐band dynamics in situ during straining experiments is presented. Various shear‐banding stages are outlined, including formation, propagation, and arrest, as well as shear‐band creep and aging. The results are discussed in a more general context of disordered materials, concluding with a summarizing overview of time‐scales involved in shear banding, and describing future research directions that may lead to controlled shear‐band plasticity in metallic glasses.

Relaxation of Bulk Metallic Glasses Studied by Mechanical Spectroscopy

The relaxational dynamics in metallic glasses (MGs) is investigated by using mechanical spectroscopy. The spectra show that in MGs there are two relaxations: (i) the α relaxation, linked to the glass transition, as observed in other classes of amorphous materials; and (ii) the β relaxation, well observed below the glass transition, with an intensity strongly dependent on the MG composition, the nature of which has been linked to the local microstructure of MGs. For the investigated MGs we find that the intensity and relaxation time of the β relaxation depends, in a reproducible fashion, on the thermal history of the samples. During aging experiments, the intensity decreases (as well as the τβ) with a time dependence described well by a stretched exponential, with an exponent β(aging) independent of the driving frequency. Moreover, we find that the activation energy Uβ and the peak temperature Tβp of the β relaxation follow the approximate relationship: Uβ ≈ 31.5RTβp (for driving frequency 1 Hz), indicating that the high temperature limit of the peak frequency is approximately the same for all the MGs investigated. Finally, the frequency separation of the α and β processes in the mechanical loss spectra for La-and Pd-based metallic glasses is tested against the prediction of the Coupling Model.

Compressed correlation functions and fast aging dynamics in metallic glasses

We present x-ray photon correlation spectroscopy measurements of the atomic dynamics in a Zr(67)Ni(33) metallic glass, well below its glass transition temperature. We find that the decay of the density fluctuations can be well described by compressed, thus faster than exponential, correlation functions which can be modeled by the well-known Kohlrausch-Williams-Watts function with a shape exponent β larger than one. This parameter is furthermore found to be independent of both waiting time and wave-vector, leading to the possibility to rescale all the correlation functions to a single master curve. The dynamics in the glassy state is additionally characterized by different aging regimes which persist in the deep glassy state. These features seem to be universal in metallic glasses and suggest a nondiffusive nature of the dynamics. This universality is supported by the possibility of describing the fast increase of the structural relaxation time with waiting time using a unique model function, independently of the microscopic details of the system.