The boson peak in metallic glasses is modeled in terms of local structural shear rearrangements. Using Eshelby's solution of the corresponding elasticity theory problem (J. D. Eshelby, Proc. Roy. Soc. A241, 376 (1957)), one can calculate the saddle point energy of such a structural rearrangement. The neighbourhood of the saddle point gives rise to soft resonant vibrational modes. One can calculate their density, their kinetic energy, their fourth order potential term and their coupling to longitudinal and transverse sound waves.
Glasses are featured with a disordered amorphous structure, being opposite to crystals that are constituted by periodic lattices. In this study we report that the exceptional thermodynamic and kinetic stability of an ultra-stable binary ZrCu metallic glass, fabricated by high-temperature physical vapor deposition, originates from ubiquitous crystal-like medium range order (MRO) constituted by Voronoi polyhedron ordering with well-defined local translational symmetry beyond nearest atomic neighbors. The crystal-like MRO significantly improves the thermodynamic and kinetic stability of the glass…
The attenuation rate of vibrational excitations in various metallic liquids and glasses has been reported to change from the quadratic dependence on wavevector at low wavevectors to the linear dependence at high wavevectors. However, the origin of this behavior is not clear. Here, the analysis of this phenomenon through molecular dynamics is presented for prototypical metallic liquids, Cu56Zr44 and Fe. It is shown that the crossover wavevector is strongly correlated with the structural coherence length characterizing coarse-grained density correlations. We suggest that the linear dependence is…
We report a wavelike fracture pattern in a Zr-based bulk metallic glass that has been deformed under quasi-static uniaxial tensions at temperatures between room temperature (300 K) and liquid nitrogen temperature (77 K). We attribute this wavelike pattern to a Kelvin-Helmholtz flow instability that occurred at certain interfaces between local cracking/softening regions. The instability criterion for the pattern formation is achieved via a hydrodynamic perturbation analysis, and furthermore an instability map is built which demonstrates that the shear velocity difference on both sides of the in…
The low temperature acoustic properties of bulk metallic glasses measured over a broad range of frequencies rigorously test the predictions of the standard tunneling model. The strength of these experiments and their analyses is mainly based on the interaction of the tunneling states with conduction electrons or quasiparticles in the superconducting state. A new series of experiments at kHz and GHz frequencies on the same sample material essentially confirms previous measurements and their discrepancies with theoretical predictions. These discrepancies can be lifted by considering more correct…
We report a strain rate (equivalent to experimental observation time) induced glass transition in model SrCaYbMg(Li)Zn(Cu) metallic glasses at room temperature. A critical strain rate, equivalent to glass transition temperature, is found for the strain rate induced a glassy state to liquid-like viscoplastic state translation. The results show that the observation time, equivalent to temperature and stress, is a key parameter for the glass transition. A three-dimension glass transition phase diagram involved in time, temperature and stress in metallic glasses is established for understanding th…
Metallic glasses response to the mechanical stress in a complex and inhomogeneous manner with plastic strain highly localized into nanoscale shear bands. Contrary to the well-defined deformation mechanism in crystalline solids, understanding the mechanical response mechanism and its intrinsic correlation with the macroscopical plasticity in metallic glasses remains long-standing issues. Through a combination of experimental and theoretical analysis, we showed that the shear banding process in metallic glasses exhibits complex chaotic dynamics, which manifests as the existence of a torus destro…
The density of vibrational states $g(ω)$ of an amorphous system is studied by using the random-matrix theory. Taking into account the most important correlations between elements of the random matrix of the system, equations for the density of vibrational states $g(ω)$ are obtained. The analysis of these equations shows that in the low-frequency region the vibrational density of states has the Debye behavior $g(ω) \sim ω^2$. In the higher frequency region, there is the boson peak as an additional contribution to the density of states. The obtained equations are in a good agreement with the num…
Studying the primary α- and secondary β-relaxation process has contributed significantly to the understanding of the structure and rheology of metallic glasses. In this letter, we report on a third relaxation mechanism indicated by a maximum in the loss modulus at low temperatures, which we term γ-relaxation. Contrary to the α- and β-relaxation mechanisms, this irreversible, low energy excitation causes a macroscopic rejuvenation, which we assign to non-affine atomic rearrangements in the matrix that are driven by thermal stresses during cooling. Observed in three different glassy alloys, the …
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…
Quantitative understanding of the fracture toughness of metallic glasses, including the associated ductile-to-brittle transitions, is not yet available. Here we use a simple model of plastic deformation in glasses, coupled to an advanced Eulerian level set formulation for solving complex free boundary problems, to calculate the fracture toughness of metallic glasses as a function of the degree of structural relaxation corresponding to different annealing times near the glass temperature. Our main result indicates the existence of an elasto-plastic crack tip instability for sufficiently relaxed…
We theoretically investigate high-pressure effects on the atomic dynamics of metallic glasses. The theory predicts compression-induced rejuvenation and the resulting strain hardening that have been recently observed in metallic glasses. Structural relaxation under pressure is mainly governed by local cage dynamics. The external pressure restricts the dynamical constraints and slows down the atomic mobility. In addition, the compression induces a rejuvenated metastable state (local minimum) at a higher energy in the free energy landscape. Thus, compressed metallic glasses can rejuvenate and the…
Micro- or minor alloying of metallic glasses is of technological interest. An originally ductile Pd-based monolithic bulk metallic glass (Pd$_{40}$Ni$_{40}$P$_{20}$) was selectively manipulated by additions of Fe or Co. The alloying effects were extreme, showing either exceptional ductility upon Co addition or immediate catastrophic failure upon Fe addition when tested under uniaxial compression or 3-point bending. The amorphous structure was characterized prior to deformation with respect to its medium-range order (MRO) using variable resolution fluctuation electron microscopy (VR-FEM). We ob…
An atomistic understanding of annealing embrittlement is a longstanding issue for metallic glasses, which is still lacking due to the insurmountable gap between the thermal history of atomic models and laboratory-made samples. Here, based on a thermal-cycling annealing method that can vary the effective quenching rate over ten orders of magnitude, we perform an atomistic study of the ductile-brittle transition in a ternary model metallic glass, which can be keyed to the annealing embrittlement in bulk metallic glasses. We reveal that thermal annealing can effectively obliterate thermally activ…
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 …
Crystallization of metallic glass as a grain-boundary nucleated process: experimental and theoretical evidence for the grain structure of metallic glasses
The discovery of magnetic and compositional effects in the low temperature properties of multi-component glasses has prompted the need to extend the standard two-level systems (2LSs) tunneling model. A possible extension \cite{Jug2004} assumes that a subset of tunneling quasi-particles is moving in a three-welled potential (TWP) associated with the ubiquitous inhomogeneities of the disordered atomic structure of the glass. We show that within an alternative, cellular description of the intermediate-range atomic structure of glasses the tunneling TWP can be fully justified. We then review how t…
Elastic flexibility, fast-ion conduction, boson and floppy modes in AgPO3-AgI glasses examined in Raman scattering, IR reflectance, MDSC, ac electrical conductivity and molar volume experiments
NOMATEN Centre of Excellence, National Center for Nuclear Research（国家核研究中心 NOMATEN 卓越中心）；Center for Complexity and Biosystems, Department of Physics "Aldo Pontremoli", University of Milan（米兰大学物理学院复杂性与生物系统中心）；Saarland University, Chair of Metallic Materials（萨尔兰大学金属材料讲席）；Glass and Time , IMFUFA, Department of Science and Environment, Roskilde University（罗斯基勒大学科学与环境学院 IMFUFA 玻璃与时间）；Department of Materials Science, Montanuniversität Leoben（莱奥本矿业大学材料科学系）；Erich Schmid Institute of Materials Science, Austrian Academy of Sciences（奥地利科学院埃里希·施密德材料科学研究所）；Department of Materials Science and Engineering, Johns Hopkins University（约翰斯·霍普金斯大学材料科学与工程系）；Department of Mechanical Engineering, Johns Hopkins University（约翰斯·霍普金斯大学机械工程系）；Department of Physics and Astronomy, Johns Hopkins University（约翰斯·霍普金斯大学物理与天文学系）；Hopkins Extreme Materials Institute, Johns Hopkins University（约翰斯·霍普金斯大学霍普金斯极端材料研究所）；Technical University of Berlin, Chair of Metallic Materials（柏林工业大学金属材料讲席）
Breakdown of material-time scaling in the microscopic dynamics of metallic glasses
Institute of Frontier Materials on Earth and in Space, German Aerospace Center（地球与太空前沿材料研究所，德国航空航天中心）；Institut Néel, Université Grenoble Alpes and Centre National de la Recherche Scientifique（内尔研究所，格勒诺布尔阿尔卑斯大学及法国国家科学研究中心）；European Synchrotron Radiation Facility（欧洲同步辐射装置）；Institute for Condensed Matter Physics, Technical University of Darmstadt（凝聚态物理研究所，达姆施塔特工业大学）；Department of Physics, Institute of Energy Technologies, Universitat Politècnica de Catalunya—BarcelonaTech（物理系，能源技术研究所，加泰罗尼亚理工大学）
Transmutation-accelerated sampling method for multi-component ZrCu(Al) metallic glasses
NOMATEN Centre of Excellence, National Center for Nuclear Research（NOMATEN卓越中心，国家核研究中心）；Univ. Lyon, INSA-Lyon, CNRS, LaMCoS, UMR 5259（里昂大学，里昂国立应用科学学院，法国国家科学研究中心，LaMCoS实验室）；Laboratoire de Mécanique des Solides, CNRS, Ecole Polytechnique（固体力学实验室，法国国家科学研究中心，巴黎综合理工学院）；Aalto University（阿尔托大学）
Structural glasses model using disorder fields: the boson peak from local ground states
Centro Brasileiro de Pesquisas Físicas（巴西物理研究中心）；Universidade Federal de Pernambuco - UFPE（伯南布哥联邦大学）；Instituto de Física Teórica, Universidade Estadual Paulista（圣保罗州立大学理论物理研究所）
We discuss a field-theoretical approach to liquids, solids and glasses, published recently [Phys.Rev.E {\bf105}, 034108 (2022)], which aims to describe these materials in a common quantum formalism. We argue that such quantum formalism is not applicable to classical liquids, and the results presented, which rely heavily on the concept of phase relaxation borrowed from quantum fluids, contradict the known hydrodynamic theory of classical liquids. In particular, the authors miss the important particle-number conservation law and the density fluctuations as hydrodynamic slow variable. Instead, th…
We report on and characterize, via molecular dynamics (MD) studies, the evolution of the structure of Cu50Zr50 and Cu64Zr36 metallic glasses (MGs) as temperature is varied. Interestingly, a percolating icosahedral network appears in the Cu64Zr36 system as it is supercooled. This leads us to introduce a static length scale, which grows dramatically as this three dimensional system approaches the glass transition. Amidst interpenetrating connections, non-interpenetrating connections between icosahedra are shown to become prevalent upon supercooling and to greatly enhance the connectivity of the …
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 present x-ray photon correlation spectroscopy measurements of the atomic dynamics in a Zr67Ni33 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.…
Using inelastic neutron scattering and molecular dynamics simulations on a model Zr-Cu-Al metallic glass, we show that transverse phonons persist well into the high-frequency regime, and can be detected at large momentum transfer. Furthermore, the apparent peak width of the transverse phonons was found to follow the static structure factor. The one-to-one correspondence, which was demonstrated for both Zr-Cu-Al metallic glass and a 3-dimensional Lennard-Jones model glass, suggests a universal correlation between the phonon dynamics and the underlying disordered structure. This remarkable corre…
Spin-charge conversion via inverse spin Hall effect (ISHE) is essential for enabling various applications of spintronics. The spin Hall response usually follows a universal scaling relation with longitudinal electric resistivity and has mild temperature dependence because elementary excitations play only a minor role in resistivity and hence ISHE. Here we report that the ISHE of metallic glasses shows nearly two orders of magnitude enhancements with temperature increase from a threshold of 80-100 K to glass transition points. As electric resistivity changes only marginally in the temperature r…
In this work we extend, review and jointly discuss earlier experiments conducted by us in hyperaged geological glasses, either in Dominican amber (20 million years old) or in Spanish amber from El Soplao (110 million years old). After characterization of their thermodynamic and elastic properties (using Differential Scanning Calorimetry around the glass-transition temperature, and measuring mass density and sound velocity), their specific heat was measured at low and very low temperatures. By directly comparing pristine amber samples (i.e. highly stabilized polymer glasses after aging for mill…
Notched bars of bulk metallic glasses, Pd$_{40}$Ni$_{40}$P$_{20}$ and Zr$_{52.5}$Cu$_{17.9}$Ni$_{14.6}$Al$_{10}$Ti$_{5}$, were deformed under 3-point bending conditions, resulting in the formation of shear bands before failure. The immediate environment of shear bands was investigated in detail using fluctuation electron microscopy to extract information on the strain-induced modifications of the medium-range order (MRO) and its lateral extension. Characteristic material-independent gradients were observed for the tensile and compressive sides of the samples indicating the impact of the local …
Magnetism prediction is of great significance for Fe-based metallic glasses (FeMGs), which have shown great commercial value. Theories or models established based on condensed matter physics exhibit several exceptions and limited accuracy. In this work, machine learning (ML) models learned from a large amount of experimental data were trained based on eXtreme gradient boosting (XGBoost), artificial neural networks (ANN), and random forest to predict the magnetic properties of FeMGs. The XGBoost and ANN models exhibited comparably excellent predictive performance, with R^2 >= 0.903, mean absolu…
The atomic theory of elasticity of amorphous solids, based on the nonaffine response formalism, is extended into the nonlinear stress-strain regime by coupling with the underlying irreversible many-body dynamics. The latter is implemented in compact analytical form using a qualitative method for the many-body Smoluchowski equation. The resulting nonlinear stress-strain (constitutive) relation is very simple, with few fitting parameters, yet contains all the microscopic physics. The theory is successfully tested against experimental data on metallic glasses, and it is able to reproduce the ubiq…
A relation between the freezing temperature ($T^{}_{\rm g}$) and the exchange couplings ($J^{}_{ij}$) in metallic spin-glasses is derived, taking the spin-correlations ($G^{}_{ij}$) into account. This approach does not involve a disorder-average. The expansion of the correlations to first order in $J^{}_{ij}/T^{}_{\rm g}$ leads to the molecular-field result from Thouless-Anderson-Palmer. Employing the current theory of the spin-interaction in disordered metals, an equation for $T^{}_{\rm g}$ as a function of the concentration of impurities is obtained, which reproduces the available data from …
We present a novel analytical model for glasses, starting from the first principle that the disorder in a glass mimics the disorder in a fluid. The origin of the boson peak is attributed to the intrinsically noncommutative geometry of the fluid disorder, which induces a van Hove singularity in the vibrational density of states. The universality of the model is exhibited by applying it to amorphous silicon, vitreous GeO$_2$ and Ba$_{8}$Ga$_{16}$Sn$_{30}$ clathrate, which show a remarkable agreement between the theoretical predictions for specific heat and the experimental data.
Boson peak, the excess low energy excitations in the terahertz regime, is one of the most unique features of disordered systems and has been linked to many anomalous properties of glass materials. The nature and structural origin of the boson peak remain elusive and have been debated for more than a half century mainly due to the lack of real-time and real-space experimental insights of the dynamic phenomenon. In this work we employed femtosecond MeV ultrafast electron diffraction to characterize the atomic dynamics of metallic glasses in real time. The experiment reveals collective atomic osc…
