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The understanding and quantification of ductility in crystalline metals, which has led to their widespread and effective usage as a structural material, is lacking in metallic glasses (MGs). Here, we introduce such a framework for ductility. This very practical framework is based on a MGs ability to support stable shear band growth, quantified in a stress gradient, gradSDB, which we measure and calculate for a range of MGs. Whether a MG behaves ductile or brittle in an application is determined by the comparison between gradsDB the applied stress field gradient, gradsapp. If gradsDB > gradsapp, the MG will behave brittle, if gradsDB < gradsapp, the MG will behave ductile, and gradsapp - gradsDB indicates how ductile. This framework can explain observed plastic properties of MGs and their apparent contradicting brittle and ductile characteristics. Looking forward, proposed framework provides the constitutive relation to quantitatively model their plastic behavior in any application, a requirement to use MGs as structural materials.

Nanofabrication techniques are limited by at least one of the required characteristics such as choice of material, control over geometry, fabrication requirements, yield, cost, and scalability. Our previously developed method of thermomechanical nanomolding fulfills these requirements, although it requires high processing temperatures. Here, we demonstrate low-temperature molding where we utilize the enhanced diffusivity on "eutectic interfaces". Gold nanorods are molded at room temperature using Au-Si alloy as feedstock. Instead of using alloy feedstock, these "eutectic interfaces" can also be established through a feedstock-mold combination. We demonstrate this by using pure Au as feedstock, which is molded into Si molds at room temperature, and also the reverse, Si feedstock is molded into Au molds forming high aspect ratio Au-Si core-shell nanorods. We discuss the mechanism of this low-temperature nanomolding in terms of lower homologous temperature at the eutectic interface. This technique, based on enhanced eutectic interface diffusion, provides a practical nanofabrication method that eliminates the previous high-temperature requirements, thereby expanding the range of the materials that can be practically nanofabricated.

The dynamics near the surface of glasses can be much faster than in the bulk. We studied the surface dynamics of a Pt-based metallic glass using electron correlation microscopy with sub-nanometer resolution. Our studies show an ∼20 K suppression of the glass transition temperature at the surface. The enhancement in surface dynamics is suppressed by coating the metallic glass with a thin layer of amorphous carbon. Parallel molecular dynamics simulations on Ni80P20 show a similar temperature suppression of the surface glass transition temperature and that the enhanced surface dynamics are arrested by a capping layer that chemically binds to the glass surface. Mobility in the near-surface region occurs via atomic caging and hopping, with a strong correlation between slow dynamics and high cage-breaking barriers and stringlike cooperative motion. Surface and bulk dynamics collapse together as a function of temperature rescaled by their respective glass transition temperatures.

The onset of yielding and the related atomic-scale plastic flow behavior of bulk metallic glasses at room temperature have not been fully understood due to the difficulty in performing the atomic-scale plastic deformation experiments needed to gain direct insight into the underlying fundamental deformation mechanisms. Here we overcome these limitations by combining a unique sample preparation method with atomic force microscopy-based indentation, which allows study of the yield stress, onset of yielding, and atomic-scale plastic flow of a platinum-based bulk metallic glass in volumes containing as little as approximately 1000 atoms. Yield stresses markedly higher than in conventional nanoindentation testing were observed, surpassing predictions from current models that relate yield stress to tested volumes; subsequent flow was then established to be homogeneous without exhibiting collective shear localization or loading rate dependence. Overall, variations in glass properties due to fluctuations of free volume are found to be much smaller than previously suggested. Metallic glasses display a high yield strength and typically deform via heterogeneous shear bands beyond the yield point. Here, deformation of as little as 1000 atoms in a Pt-based metallic glass at room temperature leads to near-theoretical yield strength, beyond which homogeneous deformation occurs.

There is a strong surge in interest for hydrogen and direct alcohol fuel cells as zero-emission energy conversion and storage devices due to their high energy density compared to that for batteries...

The glass-forming ability (GFA) of alloys, colloidal dispersions, and other particulate materials, as measured by the critical cooling rate $R_c$, can span more than ten orders of magnitude. Even after numerous previous studies, the physical features that control the GFA are still not well understood. For example, it is well-known that mixtures are better glass-formers than monodisperse systems and that particle size and cohesive energy differences among constituents improve the GFA, but it is not currently known how particle size differences couple to cohesive energy differences to determine the GFA. We perform molecular dynamics simulations to determine the GFA of equimolar, binary Lennard-Jones (LJ) mixtures versus the normalized cohesive energy difference $\epsilon_\_$ and mixing energy $\bar \epsilon_{AB}$ between particles A and B. We find several important results. First, the $\log_{10} R_c$ contours in the $\bar \epsilon_{AB}$-$\epsilon_\_$ plane are ellipsoidal for all diameter ratios, and thus $R_c$ is determined by the Mahalanobis distance $d_M$ from a given point in the $\bar \epsilon_{AB}$-$\epsilon_\_$ plane to the center of the ellipsoidal contours. Second, LJ systems for which the larger particles have larger cohesive energy are generally better glass formers than those for which the larger particles have smaller cohesive energy. Third, $d_M(\epsilon_\_,\bar \epsilon_{AB})$ is determined by the relative Voronoi volume difference between particles and local chemical order $S_{AB}$, which gives the average fraction of nearest-neighbor B particles surrounding an A particle and vice-versa. In particular, the shifted Mahalanobis distance $d_M - d^0_M$ versus the shifted chemical order $S_{AB}-S_{AB}^0$ collapses onto a hyperbolic master curve for all diameter ratios.

The realization of novel technological opportunities given by computational and autonomous materials design requires efficient and effective frameworks. For more than two decades, aflow++ (Automatic-Flow Framework for Materials Discovery) has provided an interconnected collection of algorithms and workflows to address this challenge. This article contains an overview of the software and some of its most heavily-used functionalities, including algorithmic details, standards, and examples. Key thrusts are highlighted: the calculation of structural, electronic, thermodynamic, and thermomechanical properties in addition to the modeling of complex materials, such as high-entropy ceramics and bulk metallic glasses. The aflow++ software prioritizes interoperability, minimizing the number of independent parameters and tolerances. It ensures consistency of results across property sets - facilitating machine learning studies. The software also features various validation schemes, offering real-time quality assurance for data generated in a high-throughput fashion. Altogether, these considerations contribute to the development of large and reliable materials databases that can ultimately deliver future materials systems, Comment: 47 pages, 14 figures

The transition between necking-mediated tensile failure of glasses, at elevated temperatures and/or low strain-rates, and shear-banding-mediated tensile failure, at low temperatures and/or high strain-rates, is investigated using tensile experiments on metallic glasses and atomistic simulations. We experimentally and simulationally show that this transition occurs through a sequence of macroscopic failure patterns, parametrized by the ultimate tensile strength. Quantitatively analyzing the spatiotemporal dynamics preceding failure, using large scale atomistic simulations corroborated by experimental fractography, reveals how the collective evolution and mutual interaction of shear-driven plasticity and dilation-driven void formation (cavitation) control the various macroscopic failure modes. In particular, we find that at global failure, the size of the largest cavity in the loading direction exhibits a nonmonotonic dependence on the temperature at a fixed strain rate, which is rationalized in terms of the interplay between shear- and dilation-driven plasticity. We also find that the size of the largest cavity scales with the cross-sectional area of the undeformed sample. These results shed light on tensile failure of glasses, and highlight the need to develop elasto-plastic constitutive models of glasses incorporating both shear- and dilation-driven irreversible processes.

The high entropy effect is often insufficient to fully stabilize single-phase solid solutions (SPSS), yielding only few, mostly metastable SPSS. While the prospective space of favorable SPSS formation is smaller than commonly assumed, larger degrees of metastability can open up the vast High Entropy Alloy space. We argue that HEAs form metastable SPSS through polymorphic solidification upon rapid cooling. To quantify a HEA's metastability, we propose the critical cooling rate of SPSS formation RCSPSS, analogous to RCGlass. Thereby, we can compare multicomponent alloys by their metastability and SPSS or glass forming ability, which is determined by their underlying atomic dispersity.

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.

For nanostructures in advanced electronic and plasmonic systems, a single-crystal structure with controlled orientation is essential. However, the fabrication of such devices has remained challenging, as current nanofabrication methods often suffer from either polycrystalline growth or the difficulty of integrating single crystals with substrates in desired orientations and locations to create functional devices. Here we report a thermomechanical method for the controlled growth of single-crystal nanowire arrays, which enables the simultaneous synthesis, alignment, and patterning of nanowires. Within such diffusion-based thermomechanical nanomolding (TMNM), the substrate material diffuses into nanosized cavities under an applied pressure gradient at a molding temperature of ∼0.4 times the material's melting temperature. Vertically grown face-centered cubic (fcc) nanowires with the [110] direction in an epitaxial relationship with the (110) substrate are demonstrated. The ability to control the crystal structure through the substrate takes TMNM a major step further, potentially allowing all fcc and body-centered cubic (bcc) materials to be integrated as single crystals into devices.

Description, Thermomechanical nanomolding puts a wide range of materials combinations in reach for nanofabrication., Advancements in nanotechnology require the development of nanofabrication methods for a wide range of materials, length scales, and elemental distributions. Today’s nanofabrication methods are typically missing at least one demanded characteristic. Hence, a general method enabling versatile nanofabrication remains elusive. Here, we show that, when revealing and using the underlying mechanisms of thermomechanical nanomolding, a highly versatile nanofabrication toolbox is the result. Specifically, we reveal interface diffusion and dislocation slip as the controlling mechanisms and use their transition to control, combine, and predict the ability to fabricate general materials, material combinations, and length scales. Designing specific elemental distributions is based on the relative diffusivities, the transition temperature, and the distribution of the materials in the feedstock. The mechanistic origins of thermomechanical nanomolding and their homologous temperature-dependent transition suggest a versatile toolbox capable of combining many materials in nanostructures and potentially producing any material in moldable shapes on the nanoscale.

Functional particles that respond to external stimuli are spurring technological evolution across various disciplines. While large-scale production of functional particles is needed for their use in real-life applications, precise control over particle shapes and directional properties has remained elusive for high-throughput processes. We developed a high-throughput emulsion-based process that exploits rapid vitrification of a thixotropic medium to manufacture diverse functional particles in large quantities. The vitrified medium renders stationary emulsion droplets that preserve their shape and size during solidification, and energetic fields can be applied to build programmed anisotropy into the particles. We showcase mass-production of several functional particles, including low-melting point metallic particles, self-propelling Janus particles, and unidirectionally-magnetized robotic particles, via this static-state particle fabrication process., Upscale fabrication of functionalized microparticles is a pending challenge. Here, Kim et al. exploit the rheology of a thixotropic medium to grind sizeable amounts of raw material into well-defined colloidal dispersions, physically stabilized for further production steps.

Corrosion trends in the bulk metallic glass forming alloy system Zr-Cu-Al are studied through a fast screening visual characterization method of thin film alloy libraries prepared by magnetron co-sputtering. Significant distinct brightness changes are present within the Zr-Cu-Al system when the thin film library is immersed in 3.5 wt % NaCl. Through additional quantification of corrosion current density, a correlation between change in brightness and corrosion current density is revealed, suggesting an effective rapid screening of corrosion simply by a visual method. For materials discovery with optimized multiproperties, we utilize the corrosion fast screening results and superimpose them on the composition dependence of the glass forming ability. This allows us to rapidly identify alloys with the best combination of glass forming ability and corrosion resistance, which we then confirm in bulk form.

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. Bulk metallic glasses made from alloys of iridium, nickel, tantalum and boron are developed by combinatorial methods, with higher strength at high temperature than those previously produced.

Aluminum-based quasicrystals typically form across narrow composition ranges within binary to quaternary alloys, which makes their fabrication and characterization challenging. Here, we use combinatorial approaches together with fast characterization techniques to study a wide compositional range including known quasicrystal forming compositions. Specifically, we use magnetron co-sputtering to fabricate libraries of ~140 Al-Cu-Fe and ~300 Al-Cu-Fe-Cr alloys. The alloys compositions are measured through automated energy dispersive X-ray spectroscopy. Phase formation and thermal stability are investigated for different thermal processing conditions (as-sputtered and annealed at 400 °C, 520 °C and 600 °C for Al-Cu-Fe libraries; annealed at 600 °C for Al-Cu-Fe-Cr libraries) using automated X-ray diffraction and transmission electron microscopy. In both systems the compositional regions across which the quasicrystalline phase forms are identified. In particular, we demonstrate that the quasicrystalline phase forms across an unusually broad composition range in the Al-Cu-Fe-Cr system. Additionally, some of the considered alloys vitrify during sputtering, which also allows us to study their nucleation behavior. We find that phases with polytetrahedral symmetry, such as the icosahedral quasicrystal and the λ-Al13Fe4 phase, exhibit higher nucleation rates but lower growth rates, as compared to other phases with a lower degree of polytetrahedral order. Altogether, the here used combinatorial approach is powerful to identify compositional regions of quasicrystals.

High Entropy Alloys are inherently complex and span a vast composition space, making their research and discovery challenging. Developing quantitative predictions of their phase selection requires a large quantity of consistently determined experimental data. Here, we use combinatorial methods to fabricate and characterize 2478 quinary alloys based on Al and transition metals. All data are publicly available at http://materialsatlasproject.org/ . Phase selection can be predicted for considered alloys when combining the content of FCC/BCC elements and the constituents’ atomic size difference. Mining our data reveals that High Entropy Alloys with increasing atomic size difference prefer BCC structure over FCC. This preference is typically overshadowed by other selection motifs, which dominate during close-to-equilibrium processing. Not suggested by the Hume-Rothery rules, this preference originates from the ability of the BCC structure to accommodate a large atomic size difference with lower strain energy penalty which can be practically only realized in High Entropy Alloys.

The mechanical properties of metallic glasses are often tuned by annealing, which influences these properties by adjusting the relaxation and/or crystallization status of the glasses. Here, we studied the hardness and modulus of Pt57.5Cu14.7Ni5.3P22.5 bulk metallic glass annealed at different temperatures by nanoindentation, where the annealing gives the material different fictive temperatures and fractions of crystallization. It is found that both reducing the fictive temperature of a fully amorphous sample and increasing the degree of crystallization in a partially crystallized sample increase hardness and modulus. Combining the two approaches, elevated hardness and modulus values are found for composite materials containing both crystalline and amorphous phases when they are compared to chemically identical alloys featuring similar percentages of crystalline and amorphous phases that have been prepared by annealing at higher temperatures. Our findings indicate that the mechanical properties of the platinum-based alloys can be customized by processing them with targeted heat treatments.

Discovering new metallic glasses, non-crystalline alloys with unique combinations of mechanical and chemical properties, is a challenging endeavor because it requires exploration of a vast composition space. High-throughput experiments have greatly enhanced the efficiency with which composition-dependent properties of potential glass-forming alloys can be measured, but phase identification remains a bottleneck because slow or expensive techniques such as table-top or synchrotron-based X-ray diffraction measurements are required. In this study, we developed machine learning (ML) models that can classify amorphous and crystalline phases of alloys using electrical resistivity as a primary descriptor. Artificial neural networks were constructed to correlate the electrical resistivities and the X-ray diffractograms of a broad range of combinatorially synthesized alloys. The ML models are found to classify amorphous/crystalline phases in both thin-film libraries and bulk alloys with high accuracy.

Nanomolding usually refers to a top-down fabrication method by which a formable or moldable material is shaped using a mold of nanoscale dimensions. Nanomolding is the underlying mechanism for a wide range of nanofabrication methods including template-based deposition, extrusion, nanoembossing, soft lithography, nanoimprint lithography, thermomechanical nanomolding, and nanoimprinting. Its suitability for nanofabrication in a wide range of materials and states of matter makes it one of the most versatile nanofabrication methods. It offers solutions for improving lithography techniques and the fabrication of a wide range of nanomaterials for applications including catalysts, energy, devices, and a wide range of surface functionalization. This review discusses the various physical mechanisms underlying the nanomolding process, and how they relate to the specifics of the states of matter and the material classes. Nanofabrication methods will then be categorized based on their underlying mechanism, materials that they can fabricate, and technological characteristics such as scalability, costs, precision, and versatility. This will help the reader navigate the numerous, often very specific, methods of this advanced field, and identify the most appropriate process and state of matter for a specific application. A general discussion on nanomolding follows, from accomplishments to date and the challenges that lie ahead in realizing the many potential nanodevices and structures that researchers have envisioned. Particularly the recent advances of nanomolding have resulted in a paradigm shift of nanofabrication in which the design of nanodevices is no longer limited by material and nanostructured geometries but can be selected from a very wide palette of materials.

Lead-bismuth eutectic (LBE) is a promising heat transfer fluid candidate for fast-neutron nuclear reactors and for concentrating solar power systems, due to its low melting point and advantageous thermophysical properties, but suffers from causing liquid-metal corrosion in many solids used as structural materials. Adding a suitable element to LBE to form a ternary alloy, along with proper oxygen concentration in LBE at desired temperature, might provide a formation of the protective intermetallic layers besides the formation of protective oxides on the solid surface. In this study, novel Pb-Bi-X alloys, as improvement LBE, have been designed for a broad temperature range, with X additions selected based on thermodynamic considerations and modeling, and experimentally evaluated at 700 °C. Thermodynamic calculations indicated Pb-Bi-Sb and Pb-Bi-Ge as the best candidates, and experiments provided some evidence of possible intermetallic formation of Sb with Fe-Cr-Al alloy constituents. The work pointed to the need for further research into the compatibility with structural materials at high temperatures. Keywords: Solar energy, Heat transfer, Liquid metal, Oxygen control, Fe-Cr-Al alloy

Nanoimprinting by thermoplastic forming has attracted significant attention due to its promise of low-cost fabrication of functionalized surfaces and nanostructured devices, and metallic glasses have been identified as a material class ideally suited for nanoimprinting. In particular, their featureless atomic structure suggests that there may not be an intrinsic size limit to the material’s ability to replicate a mould. Here we demonstrate atomic-scale imprinting into a platinum-based metallic glass alloy under ambient conditions using atomic step edges of a strontium titanate single crystal as a mould. The moulded metallic glass replicates the ‘atomic smoothness’ of the strontium titanate, with identical roughness to the one measured on the mould even after multiple usages and with replicas exhibiting an exceptional long-term stability of years. By providing a practical, reusable, and potentially high-throughput approach for atomic imprinting, our findings may open novel applications in surface functionalization through topographical structuring. Nanoimprinting is a technique where the surface features of a mould can be transferred onto a replica and is relevant to the production of nanostructured devices. The authors report a method that enables the imprinting of structural features of SrTiO3 single crystals at the atomic level into a replica made from bulk metallic glass.

Most of the known bulk metallic glasses lack sufficient ductility or toughness when fabricated under conditions resulting in bulk glass formation. To address this major shortcoming, processing techniques to improve ductility that mechanically affect the glass have been developed, however it remains unclear for which metallic glass formers they work and by how much. Instead of manipulating the glass state, we show here that an applied strain rate can excite the liquid, and simultaneous cooling results in freezing of the excited liquid into a glass with a higher fictive temperature. Microscopically, straining causes the structure to dilate, hence “pulls” the structure energetically up the potential energy landscape. Upon further cooling, the resulting excited liquid freezes into an excited glass that exhibits enhanced ductility. We use Zr44Ti11Cu10Ni10Be25 as an example alloy to pull bulk metallic glasses through this excited liquid cooling method, which can lead to tripling of the bending ductility. Bulk metallic glasses typically display limited ductility. Here, straining a bulk metallic glass during cooling from the supercooled region is shown to enhance bending ductility, attributed to the structure being pulled up the potential energy landscape.

Direct measurement of critical cooling rates has been challenging and only determined for a minute fraction of the reported metallic glass forming alloys. Here, we report a method that directly measures critical cooling rate of thin film metallic glass forming alloys in a combinatorial fashion. Based on a universal heating architecture using indirect laser heating and a microstructure analysis this method offers itself as a rapid screening technique to quantify glass forming ability. We use this method to identify glass forming alloys and study the composition effect on the critical cooling rate in the Al–Ni–Ge system where we identified Al51Ge35Ni14 as the best glass forming composition with a critical cooling rate of 104 K/s.

Bulk metallic glasses (BMGs) are a class of amorphous metals that exhibit high strength, ductility paired with wear and corrosion resistance. These properties suggest that they could serve as an alternative to conventional metallic implants that suffer wear and failure. In the present study, we investigated Platinum (Pt)-BMG biocompatibility in bone applications. Specifically, we investigated osteoclast formation on flat and nanopatterned Pt57.5Cu14.7Ni5.3P22.5 (atomic percent) as well as titanium (control). Specifically, receptor activator of NF-κB (RANK) ligand-induced murine bone marrow derived mononuclear cell fusion was measured on multiple nanopatterns and was found to be reduced on nanorods (80 and 200 nm in diameter) and was associated with reduced tartrate-resistant acid phosphatase (TRAP) and matrix metalloproteinase (MMP9) expression. Evaluation of mesenchymal stem cell (MSC) to osteoblast differentiation on nanopatterned Pt-BMG showed significant reduction in comparison to flat, suggesting that further exploration of nanopatterns is required to have simultaneous induction of osteoblasts and inhibition of osteoclasts.In vivo studies were also pursued to evaluate the biocompatibility of Pt-BMG in comparison to titanium. Rods of each material were implanted in the femurs of mice and evaluated by x-ray, mechanical testing, micro-computed tomography (micro-CT), and histological analysis. Overall, Pt-BMG showed similar biocompatibility with titanium suggesting that it has the potential to improve outcomes by further processing at the nanoscale.

While rhenium is an ideal material for rapid thermal cycling applications under high temperatures, such as rocket engine nozzles, its high cost limits its widespread use and prompts an exploration of viable cost-effective substitutes. In prior work, we identified a promising pool of candidate substitute alloys consisting of Mo, Ru, Ta, and W. In this work we demonstrate, based on density functional theory melting temperature calculations, that one of the candidates, Mo0.292Ru0.555Ta0.031W0.122, exhibits a high melting temperature (around 2626 K), thus supporting its use in high-temperature applications.

With its ease of implementation, low cost, high throughput, and excellent feature replication accuracy, nanoimprinting is used to fabricate structures for electrical, optical, and biological applications or to modify surface properties. If ultraprecise and/or subnanometer-sized patterns are desired, nanoimprinting has shown only limited success with polymers, silica glasses, or crystalline materials. In contrast, the absence of an intrinsic length scale that would interfere with imprinting resolution enables bulk metallic glasses (BMGs) to replicate structures down to the atomic scale through thermoplastic forming (TPF). However, only a small number of BMG-forming alloys can be used for TPF-based atomic-scale imprinting. Here, we demonstrate an alternative sputter deposition-based approach for the replication of atomic-scale features that is suited for a very broad range of amorphous alloys, thereby dramatically extending the available chemistries. Additional advantages are the method's scalability, its ability to replicate a wide range of molds, its low material consumption, and the fact that the films can readily be applied onto almost any workpiece, which together open up new avenues to atomically defined surface structuring and functionalization. Our method constitutes the advancement from proof of concept to a practical and highly versatile toolbox of atomic-scale imprinting to be explored for the science and technology of atomic-scale imprinting.