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The question of whether all materials can solidify into the glassy form proposed by Turnbull half a century ago remains unsolved. Some of the simplest systems of monatomic metals have not been vitrified, especially the close-packed face-centred cubic metals. Here we report the vitrification of gold, which is notoriously difficult to be vitrified, and several similar close-packed face-centred cubic and hexagonal metals using a method of picosecond pulsed laser ablation in a liquid medium. The vitrification occurs through the rapid cooling during laser ablation and the inhibition of nucleation by the liquid medium. Using this method, a large number of atomic configurations, including glassy configurations, can be generated simultaneously, from which a stable glass state can be sampled. Simulations demonstrate that the favourable stability of monatomic metals stems from the strong topological frustration of icosahedra-like clusters. Our work breaks the limitation of the glass-forming ability of matter, indicating that vitrification is an intrinsic property of matter and providing a strategy for the preparation and design of metallic glasses from an atomic configuration perspective.
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Since their discovery in 19601, metallic glasses based on a wide range of elements have been developed2. However, the theoretical prediction of glass-forming compositions is challenging and the discovery of alloys with specific properties has so far largely been the result of trial and error3-8. Bulk metallic glasses can exhibit strength and elasticity surpassing those of conventional structural alloys9-11, but the mechanical properties of these glasses are critically dependent on the glass transition temperature. At temperatures approaching the glass transition, bulk metallic glasses undergo plastic flow, resulting in a substantial decrease in quasi-static strength. Bulk metallic glasses with glass transition temperatures greater than 1,000 kelvin have been developed, but the supercooled liquid region (between the glass transition and the crystallization temperature) is narrow, resulting in very little thermoplastic formability, which limits their practical applicability. Here we report the design of iridium/nickel/tantalum metallic glasses (and others also containing boron) with a glass transition temperature of up to 1,162 kelvin and a supercooled liquid region of 136 kelvin that is wider than that of most existing metallic glasses12. Our Ir-Ni-Ta-(B) glasses exhibit high strength at high temperatures compared to existing alloys: 3.7 gigapascals at 1,000 kelvin9,13. Their glass-forming ability is characterized by a critical casting thickness of three millimetres, suggesting that small-scale components for applications at high temperatures or in harsh environments can readily be obtained by thermoplastic forming14. To identify alloys of interest, we used a simplified combinatorial approach6-8 harnessing a previously reported correlation between glass-forming ability and electrical resistivity15-17. This method is non-destructive, allowing subsequent testing of a range of physical properties on the same library of samples. The practicality of our design and discovery approach, exemplified by the identification of high-strength, high-temperature bulk metallic glasses, bodes well for enabling the discovery of other glassy alloys with exciting properties.
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The origin of dramatic slowing down of dynamics in metallic glass-forming liquids toward their glass transition temperatures is a fundamental but unresolved issue. Through extensive molecular dynamics simulations, here we show that, contrary to the previous beliefs, it is not local geometrical orderings extracted from instantaneous configurations but the intrinsic correlation between configurations that captures the structural origin governing slow dynamics. More significantly, it is demonstrated by scaling analyses that it is the correlation length extracted from configuration correlation rather than dynamic correlation lengths that is the key to determine the drastic slowdown of supercooled metallic liquids. The key role of the configuration correlation established here sheds important light on the structural origin of the mysterious glass transition and provides an essential piece of the puzzle for the development of a universal theoretical understanding of glass transition in glasses.
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Flexible and stretchable nanostructures have broad technological applications. Although nanostructures synthesized with metallic glasses, the alloys being of amorphous atomic structure, exhibit superior properties, they are typically too rigid to be used as flexible materials with existing synthesis techniques. In this study we report periodic and crumpled metallic glass nanostructures that can accommodate a large amount of stretching. We demonstrate that their morphologies and characteristic length scale can be well controlled, and that feature sizes as small as â¼200 nm can be readily achieved. With their integrity maintained, the nanostructures can be stretched to a strain of â¼100%, leading to broadly tunable properties. The approach is not limited to specific metallic glasses, but is applicable to a wide range of glass-forming alloys. This not only enables metallic glasses to be used under extreme stretching conditions, but also helps in the exploration of new functionalities of glassy materials.
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Although the structure and dynamics of metallic glass-forming liquids have been extensively investigated, studies of the pressure effects are rare. In the present study, the structural and dynamical properties of a ternary metallic liquid are systematically studied via extensive molecular dynamics simulations. Our results clearly show that, like isobaric cooling, isothermal compression could also slow down the dynamics of metallic liquid, leading to glass formation. However, the temperature- and pressure-induced glass transitions differ in the formation of local coordination structures and the variation of fragility. The increase of the kinetic fragility with increasing pressure is also accompanied by a monotonic structural fragility change. These findings may suggest a link between dynamics and structure. In addition, with increasing pressure, the dynamics becomes more heterogeneous, as revealed by the non-Gaussian parameter and dynamic correlation length. Here the length scales of both slow and fast domains are examined and discussed by analyzing the four-point dynamic structure factor associated with spatial correlations of atomic mobility. These correlation lengths coexist in the metallic liquids and grow comparatively in the considered temperature and pressure ranges. Finally, the scaling relation between the relaxation times and correlation lengths is discussed, which is found to be consistent with the spirit of Adam-Gibbs and random first-order transition theories.
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A ternary metallic glass-forming liquid is found to be not strongly correlating thermodynamically, but its average dynamics, dynamic heterogeneities including the high order dynamic correlation length, and static structure are still well described by thermodynamic scaling with the same scaling exponent γ. This may indicate that the metallic liquid could be treated as a single-parameter liquid. As an intrinsic material constant stemming from the fundamental interatomic interactions, γ is theoretically predicted from the thermodynamic fluctuations of the potential energy and the virial. Although γ is conventionally understood merely from the repulsive part of the inter-particle potentials, the strong correlation between γ and the Grüneisen parameter up to the accuracy of the Dulong-Petit approximation demonstrates the important roles of anharmonicity and attractive force of the interatomic potential in governing glass transition of metallic glassformers. These findings may shed light on how to understand metallic glass formation from the fundamental interatomic interactions.
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The topological Hall effect (THE) is the transport response of chiral spin textures and thus can serve as a powerful probe for detecting and understanding these unconventional magnetic orders. So far, the THE is only observed in either noncentrosymmetric systems where spin chirality is stabilized by Dzyaloshinskii-Moriya interactions, or triangular-lattice magnets with Ruderman-Kittel-Kasuya-Yosida-type interactions. Here, a pronounced THE is observed in a Fe-Co-Ni-Mn chemically complex alloy with a simple face-centered cubic (fcc) structure across a wide range of temperatures and magnetic fields. The alloy is shown to have a strong magnetic frustration owing to the random occupation of magnetic atoms on the close-packed fcc lattice and the direct Heisenberg exchange interaction among atoms, as evidenced by the appearance of a reentrant spin glass state in the low-temperature regime and the first principles calculations. Consequently, THE is attributed to the nonvanishing spin chirality created by strong spin frustration under the external magnetic field, which is distinct from the mechanism responsible for the skyrmion systems, as well as geometrically frustrated magnets.
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High saturation magnetic flux density (Bs ) of soft magnetic materials is essential for increasing the power density of modern magnetic devices and motor machines. Yet, increasing Bs is always at the expense of high coercivity (Hc ), presenting a general trade-off in the soft magnetic material family. Here, superior comprehensive soft magnetic properties, i.e., an exceptionally high Bs of up to 1.94 T and Hc as low as 4.3 A m-1 are unprecedentedly combined in an FeCo-based alloy. This alloy is obtained through a composition design strategy to construct a transitional microstructure between amorphous and traditional nanocrystalline alloys, with nanocrystals (with < 5 nm-sized crystal-like regions around) sparsely dispersed in an amorphous matrix. Such transitional microstructure possesses extremely low magnetic anisotropy caused by the annihilation of quasi-dislocation dipoles, and a strong magnetic exchange interaction, which leads to excellent comprehensive magnetic properties. The results provide useful guidelines for the development of the next generation of soft magnetic materials, which are promising for applications of high-frequency, high-efficiency, and energy-saving devices.
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How glasses relax at room temperature is still a great challenge for both experimental and simulation studies due to the extremely long relaxation time-scale. Here, by employing a modified molecular dynamics simulation technique, we extend the quantitative measurement of relaxation process of metallic glasses to room temperature. Both energy relaxation and dynamics, at low temperatures, follow a stretched exponential decay with a characteristic stretching exponent ß = 3/7, which is distinct from that of supercooled liquid. Such aging dynamics originates from the release of energy, an intrinsic nature of out-of-equilibrium system, and manifests itself as the elimination of defects through localized atomic strains. This finding is also supported by long-time stress-relaxation experiments of various metallic glasses, confirming its validity and universality. Here, we show that the distinct relaxation mechanism can be regarded as a direct indicator of glass transition from a dynamic perspective.
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Physical aging is a long-lasting research hot spot in the glass community, yet its long-term effects remain unclear because of the limited experimental time. In this study, we discover the extraordinary aging effects in five typical lunar glassy particles with diameters ranging from about 20 to 53 micrometers selected from Chang'e-5 lunar regolith. It is found that geological time scales' aging can lead to unusually huge modulus enhancements larger than 73.5% while much weaker effects on hardness (i.e., varies decoupling evolutions of Young's modulus and hardness during aging) in these lunar glassy samples. Such extraordinary aging effects are primarily attributed to the natural selected complex glassy compositions and structures, consistent with high entropy and minor element doping criteria, prevailing under the special lunar conditions and the extensive aging time for the lunar glasses. This study offers valuable insights for developing high-performance and stable glassy materials for radiation protection and advanced space explorations.
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Lunar glasses with different origins act as snapshots of their formation processes, providing a rich archive of the Moon's formation and evolution. Here, we reveal diverse glasses from Chang'E-5 (CE-5) lunar regolith, and clarify their physical origins of liquid quenching, vapor deposition and irradiation damage respectively. The series of quenched glasses, including rotation-featured particles, vesicular agglutinates and adhered melts, record multiple-scale impact events. Abundant micro-impact products, like micron- to nano-scale glass droplets or craters, highlight that the regolith is heavily reworked by frequent micrometeorite bombardment. Distinct from Apollo samples, the indigenous ultra-elongated glass fibers drawn from viscous melts and the widespread ultra-thin deposited amorphous rims without nanophase iron particles both indicate a relatively gentle impact environment at the CE-5 landing site. The clarification of multitype CE-5 glasses also provides a catalogue of diverse lunar glasses, meaning that more of the Moon's mysteries, recorded in glasses, could be deciphered in future.
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The prevalence of wide-bandgap (WBG) semiconductors allows modern electronic devices to operate at much higher frequencies. However, development of soft magnetic materials with high-frequency properties matching the WBG-based devices remains challenging. Here, a promising nanocrystalline-amorphous composite alloy with a normal composition Fe75.5 Co0.5 Mo0.5 Cu1 Nb1.5 Si13 B8 in atomic percent is reported, which is producible under industrial conditions, and which shows an exceptionally high permeability at high frequencies up to 36 000 at 100 kHz, an increase of 44% compared with commercial FeSiBCuNb nanocrystalline alloy (25 000 ± 2000 at 100 kHz), outperforming all existing nanocrystalline alloy systems and commercial soft magnetic materials. The alloy is obtained by a unique magnetic-heterogeneous nanocrystallization mechanism in an iron-based amorphous alloy, which is different from the traditional strategy of nanocrystallization by doping nonmagnetic elements (e.g., Cu and Nb). The induced magnetic inhomogeneity by adding Co atoms locally promotes the formation of highly ordered structures acting as the nuclei of nanocrystals, and Mo atoms agglomerate around the interfaces of the nanocrystals, inhibiting nanocrystal growth, resulting in an ultrafine nanocrystalline-amorphous dual-phase structure in the alloy. The exceptional soft magnetic properties are shown to be closely related to the low magnetic anisotropy and the unique spin rotation mechanism under alternating magnetic fields.
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The G-phase, a new metastable phase with its potential energy sitting right in the middle of the glass and crystal, was recently discovered in some simulations when the molten metallic liquid was quenched down to room temperature. In comparison with ordinary glass, the G-phase has a more ordered short-range structure but a similarly disordered long-range structure. The question is whether the G-phase can be termed a new type of glass. In this work, G-phase Cu is made in a molecular dynamics simulation using rapid quenching or isothermal annealing. Weak oscillations are found in the long-range atomic structure. The pseudo-fictive temperature is significantly lower than the Kauzmann temperature; fivefold twinning structures are distinguished in the G-phase whose constituent atoms are face-center-cubic or hexagonal-cubic-packed. This evidence suggests that G-phase Cu is not a glass. However, the G-phase is also metastable against crystallization. Therefore, G-phase Cu is neither a glass nor a crystal but belongs to a new mesophase.
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Glasses have markedly different stability around their glass transition temperature (Tg), and metallic glasses (MGs) are conventionally regarded as metastable compared to other glasses such as silicate glass or amber. Here, we show an aging experiment on a Ce-based MG around its Tg (~0.85Tg) for more than 17 years. We find that the MG with strong fragility could transform into kinetic and thermodynamic hyperstable state after the long-term room temperature aging and exhibits strong resistance against crystallization. The achieved hyperstable state is closer to the ideal glass state compared with that of other MGs and similar to that of the million-year-aged amber, which is attributed to its strong fragility and strong resistance against nucleation. It is also observed through the asymmetrical approaching experiment that the hyperaged Ce-based MG can reach equilibrium liquid state below Tg without crystallization, which supports the idea that nucleation only occurs after the completion of enthalpy relaxation.
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Metallic Mimosa pudica, a three-dimensional (3D) biomimetic structure made of metallic glass, is formed via laser patterning: Blooming, closing, and reversing of the metallic M. pudica can be controlled by an applied magnetic field or by manual reshaping. An array of laser-crystallized lines is written in a metallic glass ribbon. Changes in density and/or elastic modulus due to laser patterning result in an appropriate size mismatch between the shrunken crystalline regions and the glassy matrix. The residual stress and elastic distortion energy make the composite material to buckle within the elastic limit and to obey the minimum elastic energy criterion. This work not only provides a programming route for constructing buckling structures of metallic glasses but also provides clues for the study of materials with automatic functions desired in robotics, electronic devices, and, especially, medical devices in the field of medicine, such as vessel scaffolds and vascular filters, which require contactless expansion and contraction functions.
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Stretchable electrodes are essential components for wearable electronics. However, the stretchability of the electrodes is often achieved with the sacrifice of electronic conductivity along with huge variation in resistance. In this work, stretchable metallic glass electrodes (MG-electrodes) that have both high electronic conductivity and excellent electronic stability are developed. The stretchability of the MG-electrode is significantly improved by shrinking MG films deposited on substrates with pre-strain. We demonstrate two types of MG-electrodes. One is a transparent MG-electrode for uniaxial stretching, and the other with better conductivity is for biaxial stretching. Compared with previous electrodes, the MG-electrodes exhibit a combination of high conductivity and negligible resistivity change (<5%), making them promising candidates for interconnections. Along with the excellent corrosion resistance of metallic glasses, the electrodes may be used in harsh environments.
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Crack propagation is the major vehicle for material failure, but the mechanisms by which cracks propagate remain longstanding riddles, especially for glassy materials with a long-range disordered atomic structure. Recently, cavitation was proposed as an underlying mechanism governing the fracture of glasses, but experimental determination of the cavitation behavior of fracture is still lacking. Here, we present unambiguous experimental evidence to firmly establish the cavitation mechanism in the fracture of glasses. We show that crack propagation in various glasses is dominated by the self-organized nucleation, growth, and coalescence of nanocavities, eventually resulting in the nanopatterns on the fracture surfaces. The revealed cavitation-induced nanostructured fracture morphologies thus confirm the presence of nanoscale ductility in the fracture of nominally brittle glasses, which has been debated for decades. Our observations would aid a fundamental understanding of the failure of disordered systems and have implications for designing tougher glasses with excellent ductility.
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By decreasing the rate of physical vapor deposition, ZrCuAl metallic glasses with improved stability and mechanical performances can be formed, while the microscopic structural mechanisms remain unclear. Here, with scanning transmission electron microscopy and high-energy synchrotron X-ray diffraction, we found that the metallic glass deposited at a higher rate exhibits a heterogeneous structure with compositional fluctuations at a distance of a few nanometers, which gradually disappear on decreasing the deposition rate; eventually, a homogeneous structure is developed approaching ultrastability. This microscopic structural evolution suggests the existence of the following two dynamical processes during ultrastable metallic glass formation: a faster diffusion process driven by the kinetic energy of the depositing atoms, which results in nanoscale compositional fluctuations, and a slower collective relaxation process that eliminates the compositional and structural heterogeneity, equilibrates the deposited atoms, and strengthens the local atomic connectivity.
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Determination and conceptualization of atomic structures of metallic glasses or amorphous alloys remain a grand challenge. Structural models proposed for bulk metallic glasses are still controversial owing to experimental difficulties in directly imaging the atom positions in three-dimensional structures. With the advanced atomic-resolution imaging, here we directly observed the atomic arrangements in atomically thin metallic glassy membranes obtained by vapor deposition. The atomic packing in the amorphous membrane is shown to have a fractal characteristic, with the fractal dimension depending on the atomic density. Locally, the atomic configuration for the metallic glass membrane is composed of many types of polygons with the bonding angles concentrated on 45°-55°. The fractal atomic structure is consistent with the analysis by the percolation theory, and may account for the enhanced relaxation dynamics and the easiness of glass transition as reported for the thin metallic glassy films or glassy surface.