The atomic-scale structural rearrangement of glasses on applied stress is central to the understanding of their macroscopic mechanical properties and behaviour. However, experimentally resolving the atomic-scale structural changes of a deformed glass remains challenging due to the disordered nature of the glass structure. Conventional structural analyses such as X-ray diffraction are based on the assumption of structural isotropy and hence cannot discern the subtle atomic-scale structural rearrangement induced by deformation. Here we show that structural anisotropy correlates with non-affine atomic displacements-meaning those that do not preserve parallel lines in the atomic structure-in various types of glass. This serves as an approach for identifying the atomic-scale non-affine deformation in glasses. We also uncover the atomic-level mechanism responsible for plastic flow, which differs between metallic glasses and covalent glasses. The non-affine structural rearrangements in metallic glasses are mediated through the stretching or contraction of atomic bonds. The non-affinity of covalent glasses that occurs in a less localized manner is mediated through the rotation of atomic bonds or chains without changing the bond length. These findings provide key ingredients for exploring the atomic-scale process governing the macroscopic deformation of amorphous solids. Resolving the structural changes of a deformed glass on the atomic scale is challenging due to its disordered nature. Now, high-energy diffraction measurements show that non-line-preserving atomic displacements in glasses correlate with structural anisotropy.

X-ray photon correlation spectroscopy (XPCS) allows for the resolution of dynamic processes within a material across a wide range of length and time scales. X-ray speckle visibility spectroscopy (XSVS) is a related method that uses a single diffraction pattern to probe ultrafast dynamics. Interpretation of the XPCS and XSVS data in terms of underlying physical processes is necessary to establish the connection between the macroscopic responses and the microstructural dynamics. To aid the interpretation of the XPCS and XSVS data, we present a computational framework to model these experiments by computing the X-ray scattering intensity directly from the atomic positions obtained from molecular dynamics (MD) simulations. We compare the efficiency and accuracy of two alternative computational methods: the direct method computing the intensity at each diffraction vector separately, and a method based on fast Fourier transform that computes the intensities at all diffraction vectors at once. The computed X-ray speckle patterns capture the density fluctuations over a range of length and time scales and are shown to reproduce the known properties and relations of experimental XPCS and XSVS for liquids.

The origin of limited plasticity in metallic glasses is elusive, with no apparent link to their atomic structure. We propose that the response of the glassy structure to applied stress, not the original structure itself, provides a gauge to predict the degree of plasticity. We carried out high-energy x-ray diffraction on various bulk metallic glasses (BMGs) under uniaxial compression within the elastic limit and evaluated the anisotropic pair distribution function. We show that the extent of local deviation from the affine (uniform) deformation in the elastic regime is strongly correlated with the plastic behavior of BMGs beyond yield, across chemical compositions and sample history. The results suggest that the propensity for collective local atomic rearrangements under stress promotes plasticity.

Experimentally resolving atomic-scale structural changes of a deformed glass remains challenging owing to the disordered nature of glass structure. Here, we show that the structural anisotropy emerges as a general hallmark for different types of glasses (metallic glasses, oxide glass, amorphous selenium, and polymer glass) after thermo-mechanical deformation, and it is highly correlates with local nonaffine atomic displacements detected by the high-energy X-ray diffraction technique. By analyzing the anisotropic pair density function, we unveil the atomic-level mechanism responsible for the plastic flow, which notably differs between metallic glasses and covalent glasses. The structural rearrangements in metallic glasses are mediated through cutting and formation of atomic bonds, which occurs in some localized inelastic regions embedded in elastic matrix, whereas that of covalent glasses is mediated through the rotation of atomic bonds or chains without bond length change, which occurs in a less localized manner.

Zr-based metallic glasses are prepared by quenching supercooled liquid under pressure. These glasses are stable in ambient conditions after decompression. The High Pressure Quenched glasses have a distinct structure and properties. The pair distribution function shows redistribution of the Zr-Zr interatomic distances and their shift towards smaller values. These glasses exhibit higher density, hardness, elastic modulus, and yield stress. Upon heating at ambient pressure, they show volume expansion and distinct relaxation behavior, reaching an equilibrated state above the glass transition. These experimental results are consistent with an idea of pressure-induced low to high density liquid transition in the supercooled melt.

Discovery of anti-sintering noble metal catalysts is challenging, as supported noble metal species tend to aggregate at high temperatures, leading to severely deteriorated catalytic performances. Here we show that 1 wt% of noble metal species including Au, Pd and Ru can be incorporated into high-entropy oxides (HEOs) through entropy stabilization at 900 °C in air. A reversible temperature-dependent dissolution-exsolution process is observed for Au-HEO. Further correlation with distinct CO oxidation capabilities demonstrates the potential to utilize the entropy effect to access self-regenerative catalysts for catalytic reactions.

A wide range of behaviors, including non-monotonic rejuvenation and relaxation, and the ability to qualitatively change the effect by varying the structural state of the glass was observed during thermal cycling of bulk metallic glasses. For this, we considered various bulk metallic glasses, Zr44Ti11Cu10Ni10Be25, Pd43Cu27Ni10P20, Pt57.5Cu14.7Ni5.3P22.5, and La55Al25Ni20, at various fictive temperatures to study the effect of thermal cycling on structure, thermal signature, and fracture toughness. For some BMGs and conditions considered here, thermal cycling results in a looser structure and an increase in fracture toughness. We found that for certain other BMGs and conditions, thermal cycling results in relaxation, reflected in a denser structure, and a decrease in fracture toughness. All these responses are non-monotonic and reveal a pronounced extremum with fracture toughness values of ± 50% of the original value, before approaching a value similar to the original value prior to thermal cycling. Such richness in response to thermal cycling suggests incompleteness of the previous picture where monotonically decreasing local stresses resulting in a homogenization of the structure with increasing cycle number. Our finding suggests that relative comparisons of various contributions including activation barriers for α-relaxation have to be considered which are also constantly changing, to decide if further cycling results in an increase or a decrease in fracture toughness. The fracture toughness’ response to thermal cycling can be correlated with the average atomic structures’ response to thermal cycling, while the thermal response does not exhibit an obvious correlation.

Using high energy X-ray diffraction, we study the phase transition from α to ω in Zr via high-pressure torsion. We examine the evolution of the texture and establish the crystallographic orientation relationship between the α and ω phases. The orientation relationship supports the Silcock/Rabinkim direct transformation pathway and excludes the possibility of transition through the intermediate β phase, the Usikov/Zilbershtein pathway. The texture development in both α and ω phases of Zr during high-pressure torsion is quantified and explained in terms of the dominant slip system and the orientation relationship during martensitic transformation.

The fracture toughness of glassy materials remains poorly understood. In large part, this is due to the disordered, intrinsically non-equilibrium nature of the glass structure, which challenges its theoretical description and experimental determination. We show that the notch fracture toughness of metallic glasses exhibits an abrupt toughening transition as a function of a well-controlled fictive temperature (Tf), which characterizes the average glass structure. The ordinary temperature, which has been previously associated with a ductile-to-brittle transition, is shown to play a secondary role. The observed transition is interpreted to result from a competition between the Tf-dependent plastic relaxation rate and an applied strain rate. Consequently, a similar toughening transition as a function of strain rate is predicted and demonstrated experimentally. The observed mechanical toughening transition bears strong similarities to the ordinary glass transition and explains the previously reported large scatter in fracture toughness data and ductile-to-brittle transitions.