arXiv subjects

Jan Schroers

Publications and source records attributed to Jan Schroers.

At least 19 recordsLinked to original sources

arXiv2025

Computational Study of Density Fluctuation-Induced Shear Bands Formation in Bulk Metallic Glasses

Seemingly identical Bulk Metallic Glasses (BMG) often exhibit strikingly different mechanical properties despite having the same composition and fictive temperature. A postulated mechanism underlying these differences is the presence of "defects". Here we investigate this hypothesis through the study of the effect of density fluctuations on shear band formation under an applied stress. We find that the critical shear stress is strongly dependent on the magnitude and size of the fluctuations. This finding also elucidates why, historically, critical shear stresses obtained in simulations have differed so much from those found experimentally, as typical simulations setups might favor unrealistically uniform geometries.

cond-mat.dis-nn↗

arXiv2025

Soliquidy: a descriptor for atomic geometrical confusion

Tailoring material properties often requires understanding the solidification process. Herein, we introduce the geometric descriptor Soliquidy, which numerically captures the Euclidean transport cost between the translationally disordered versus ordered states of a materials. As a testbed, we apply Soliquidy to the classification of glass-forming metal alloys. By extending and combining an experimental library of metallic thin-films (glass/no-glass) with the aflow.org computational database (geometrical and energetic information of mixtures) we found that the combination of Soliquity and formation enthalpies generates an effective classifier for glass formation. Such classifier is then used to tackle a public dataset of metallic glasses showing that the glass-agnostic assumptions of Soliquity can be useful for understanding kinetically-controlled phase transitions.

cond-mat.mtrl-sci↗

arXiv2024

Nano-Patterned Pt-Based Metallic Glass Electrocatalysts with In-Situ Copper Oxide Foam for Enhanced Hydrogen Evolution

Hydrogen is a promising energy carrier for replacing fossil fuels, and hydrogen production via hydrogen evolution reaction (HER) is an environmentally friendly option if electrocatalysts with low overpotentials and long-term stability are used. In this work, the electrocatalytic performance of $\mathrm{Pt_{57.5}Cu_{14.7}Ni_{5.3}P_{22.5}}$ bulk metallic glass (BMG) with flat, micro-patterned, and nano-patterned surfaces for HER in 0.5 M H2SO4 is studied. The nano-patterned Pt-BMG demonstrates outstanding long-term stability and self-improving behavior with a final overpotential of 150 mV and a Tafel slope of 42 $\mathrm{mV dec^{-1}}$ after 1000 linear sweep voltammetry (LSV) cycles, which is respectively 42% and 37% lower than in the first LSV cycle. X-ray photoelectron spectroscopy (XPS) and Auger electron spectroscopy (AES) indicate the formation of a layer of CuO/Cu2O foam deposited on top of the nano-patterned surface during the stability test of 1000 LSV cycles. A three-step process is proposed to explain the formation of CuxO foam via dynamic hydrogen bubble templating (DHBT) electrodeposition from Cu dissolution of the Pt-BMG without using copper salt. This work provides a method to create CuxO foams that could be used for various applications. Moreover, nano-patterned BMGs with DHBT deposition offer a feasible strategy to synthesize metal or metal-oxide foams.

cond-mat.mtrl-sci↗

arXiv2023

A Framework for Ductility in Metallic Glasses

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.

cond-mat.mtrl-sci↗

arXiv2023

Bridging necking and shear-banding mediated tensile failure in glasses

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.

cond-mat.mtrl-sci↗

arXiv2023

Special Glass Structures for First Principles Studies of Bulk Metallic Glasses

The atomic-level structure of bulk metallic glasses is a key determinant of their properties. An accurate representation of amorphous systems in computational studies has traditionally required large supercells that are unfortunately computationally demanding to handle using the most accurate ab initio calculations. To address this, we propose to specifically design small-cell structures that best reproduce the local geometric descriptors (e.g., pairwise distances or bond angle distributions) of a large-cell simulation. We rely on molecular dynamics (MD) driven by empirical potentials to generate the target descriptors, while we use reverse Monte Carlo (RMC) methods to optimize the small-cell structure. The latter can then be used to determine mechanical and electronic properties using more accurate electronic structure calculations. The method is implemented in the Metallic Amorphous Structures Toolkit (MAST) software package.

cond-mat.mtrl-sci↗

arXiv2023

Characterizing the mechanical response of metallic glasses to uniaxial tension using a spring network model

Metallic glasses are frequently used as structural materials. Therefore, it is important to develop methods to predict their mechanical response as a function of the microstructure prior to loading. We develop a coarse-grained spring network model, which describes the mechanical response of metallic glasses using an equivalent series network of springs, which can break and re-form to mimic atomic rearrangements during deformation. To validate the model, we perform simulations of quasistatic, uniaxial tension of Lennard-Jones and embedded atom method (EAM) potentials for Cu$_{50}$Zr$_{50}$ metallic glasses. We consider samples prepared using a wide range of cooling rates and with different amounts of crystalline order. We show that both the Lennard-Jones and EAM models possess qualitatively similar stress $σ$ versus strain $γ$ curves. By specifying five parameters in the spring network model (ultimate strength, strain at ultimate strength, slopes of $σ(γ)$ at $γ=0$ and at large strain, and strain at fracture where $σ=0$), we can accurately describe the form of the stress-strain curves during uniaxial tension for the computational studies of Cu$_{50}$Zr$_{50}$, as well as recent experimental studies of several Zr-based metallic glasses. For the computational studies of Cu$_{50}$Zr$_{50}$, we find that the yield strain distribution is shifted to larger strains for slowly cooled glasses compared to rapidly cooled glasses. In addition, the average number of new springs and their rate of formation decreases with decreasing cooling rate. These effects offset each other at large strains, causing the stress-strain curve to become independent of the sample preparation protocol in this regime. In future studies, we will extract the parameters that define the spring network model directly from atomic rearrangements that occur during uniaxial deformation.

cond-mat.mtrl-sci↗

arXiv2022

The glass-forming ability of binary Lennard-Jones systems

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 $ε_\_$ and mixing energy $\bar ε_{AB}$ between particles A and B. We find several important results. First, the $\log_{10} R_c$ contours in the $\bar ε_{AB}$-$ε_\_$ 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 $\bar ε_{AB}$-$ε_\_$ 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, $d_M(ε_\_,\bar ε_{AB})$ 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.

cond-mat.mtrl-sci↗

arXiv2020

Glass formation in binary alloys with different atomic symmetries

Prediction of the glass forming ability (GFA) of alloys remains a major challenge. We are not able to predict the composition dependence of the GFA of even binary alloys. To investigate the effect of each element's propensity to form particular crystal structures on glass formation, we focus on binary alloys composed of elements with the same size, but different atomic symmetries using the patchy-particle model. For mixtures with atomic symmetries that promote different crystal structures, the minimum critical cooling rate $R_c$ is only a factor of $5$ lower than that for the pure substances. For mixtures with different atomic symmetries that promote local crystalline and icosahedral order, the minimum $R_c$ is more than $3$ orders of magnitude lower than that for pure substances. Results for $R_c$ for the patchy-particle model are in agreement with those from embedded atom method simulations and sputtering experiments of NiCu, TiAl, and high entropy alloys.

cond-mat.mtrl-sci↗

arXiv2019

Intrinsic dissipation mechanisms in metallic glass resonators

Micro- and nano-resonators have important applications including sensing, navigation, and biochemical detection. Their performance is quantified using the quality factor $Q$, which gives the ratio of the energy stored to the energy dissipated per cycle. Metallic glasses are a promising materials class for micro- and nano-scale resonators since they are amorphous and can be fabricated precisely into complex shapes on these lengthscales. To understand the intrinsic dissipation mechanisms that ultimately limit large $Q$-values in metallic glasses, we perform molecular dynamics simulations to model metallic glass resonators subjected to bending vibrations. We calculate the vibrational density of states, redistribution of energy from the fundamental mode of vibration, and $Q$ versus the kinetic energy per atom $K$ of the excitation. In the linear and nonlinear response regimes where there are no atomic rearrangements, we find that $Q \rightarrow \infty$ (since we do not consider coupling to the environment). We identify a characteristic $K_r$ above which atomic rearrangements occur, and there is significant energy leakage from the fundamental mode to higher frequencies, causing finite $Q$. Thus, $K_r$ is a critical parameter determining resonator performance. We show that $K_r$ decreases as a power-law, $K_r\sim N^{-k},$ with increasing system size $N$, where $k \approx 1.3$. We estimate the critical strain $\langle γ_r \rangle \sim 10^{-8}$ for micron-sized resonators below which atomic rearrangements do not occur, and thus large $Q$-values can be obtained when they are operated below $γ_r$. We find that $K_r$ for amorphous resonators is comparable to that for resonators with crystalline order.

cond-mat.mtrl-sci↗

arXiv2019

Tuning the glass-forming ability of metallic glasses through energetic frustration

The design of multi-functional BMGs is limited by the lack of a quantitative understanding of the variables that control the glass-forming ability (GFA) of alloys. Both geometric frustration (e.g. differences in atomic radii) and energetic frustration (e.g. differences in the cohesive energies of the atomic species) contribute to the GFA. We perform molecular dynamics simulations of binary Lennard-Jones mixtures with only energetic frustration. We show that there is little correlation between the heat of mixing and critical cooling rate $R_c$, below which the system crystallizes, except that $ΔH_{\rm mix} < 0$. By removing the effects of geometric frustration, we show strong correlations between $R_c$ and the variables $ε_- = (ε_{BB}-ε_{AA})/(ε_{AA}+ε_{BB})$ and ${\overline ε}_{AB} = 2ε_{AB}/(ε_{AA}+ε_{BB})$, where $ε_{AA}$ and $ε_{BB}$ are the cohesive energies of atoms $A$ and $B$ and $ε_{AB}$ is the pair interaction between $A$ and $B$ atoms. We identify a particular $f_B$-dependent combination of $ε_-$ and ${\overline ε}_{AB}$ that collapses the data for $R_c$ over nearly $4$ orders of magnitude in cooling rate.

cond-mat.mtrl-sci↗

arXiv2018

Spatially Heterogeneous Dynamics in a Metallic Glass Forming Liquid Imaged by Electron Correlation Microscopy

Supercooled liquids exhibit spatial heterogeneity in the dynamics of their fluctuating atomic arrangements. The length and time scales of the heterogeneous dynamics are central to the glass transition and influence nucleation and growth of crystals from the liquid. We report direct experimental visualization of the spatially heterogeneous dynamics as a function of temperature in the supercooled liquid state of a Pt-based metallic glass, using electron correlation microscopy with sub-nanometer resolution. An experimental four point space-time intensity correlation function demonstrates a growing dynamic correlation length, $ξ$, upon cooling of the liquid toward the glass transition temperature. $ξ$ as a function of the relaxation time $τ$ data are in the good agreement with the Adam-Gibbs, inhomogeneous mode coupling theory and random first order transition theory of the glass transition. The same experiments demonstrate the existence of a nanometer thickness near surface layer with order of magnitude shorter relaxation time than inside the bulk.

cond-mat.mtrl-sci↗

arXiv2017

Particle rearrangement and softening contributions to the nonlinear mechanical response of glasses

Amorphous materials such as metallic, polymeric, and colloidal glasses, exhibit complex preparation-dependent mechanical response to applied shear. We perform numerical simulations to investigate the mechanical response of binary Lennard-Jones glasses undergoing athermal, quasistatic pure shear as a function of the cooling rate $R$ used to prepare them. The ensemble-averaged stress versus strain curve $\langleσ(γ)\rangle$ resembles the spatial average in the large size limit, which appears smooth and displays a putative elastic regime at small strains, a yielding-related peak at intermediate strain, and a plastic flow regime at large strains. In contrast, for each glass configuration in the ensemble, the stress-strain curve consists of many short nearly linear segments that are punctuated by particle-rearrangement-induced rapid stress drops. We quantify the shape of the small stress-strain segments, as well as the frequency and size of the stress drops in each glass configuration. We decompose the stress loss into the loss from particle rearrangements and from softening i.e., the reduction of the slopes of the linear segments in $σ(γ)$), and then compare the two contributions as a function of $R$ and $γ$. For the current studies, the rearrangement-induced stress loss is larger than the softening-induced stress loss, however, softening stress losses increase with decreasing cooling rate. We also characterize the structure of the potential energy landscape along the strain direction for glasses prepared with different $R$, and observe a dramatic change of the properties of the landscape near the yielding transition. We then show that the rearrangement-induced energy loss per strain can serve as an order parameter for the yielding transition, which sharpens for slow cooling rates and in the large system-size limit.

cond-mat.stat-mech↗

arXiv2016

Spectral descriptors for bulk metallic glasses based on the thermodynamics of competing crystalline phases

Metallic glasses have attracted considerable interest in recent years due to their unique combination of superb properties and processability. Predicting bulk metallic glass formers from known parameters remains a challenge and the search for new systems is still performed by trial and error. It has been speculated that some sort of "confusion" during crystallization of the crystalline phases competing with glass formation could play a key role. Here, we propose a heuristic descriptor quantifying confusion and demonstrate its validity by detailed experiments on two well-known glass forming alloy systems. With the insight provided by these results, we develop a robust model for predicting glass formation ability based on the spectral decomposition of geometrical and energetic features of crystalline phases calculated ab-initio in the AFLOW high throughput framework. Our findings indicate that the formation of metallic glass phases could be a much more common phenomenon than currently estimated, with more than 17% of binary alloy systems being potential glass formers. Our approach is capable of pinpointing favorable compositions, overcoming a major bottleneck hindering the discovery of new materials. Hence, it is demonstrated that smart descriptors, based solely on the energetics and structure of competing crystalline phases calculated from first-principles and available in online databases, others the sought-after key for accelerated discovery of novel metallic glasses.

cond-mat.mtrl-sci↗

arXiv2016

The effects of cooling rate on particle rearrangement statistics: Rapidly cooled glasses are more ductile and less reversible

Amorphous solids, such as metallic, polymeric, and colloidal glasses, display complex spatiotemporal response to applied deformations. In contrast to crystalline solids, during loading, amorphous solids exhibit a smooth crossover from elastic response to plastic flow. In this study, we investigate the mechanical response of binary Lennard-Jones glasses to athermal, quasistatic pure shear as a function of the cooling rate used to prepare them. We find several key results concerning the connection between strain-induced particle rearrangements and mechanical response. We show that more rapidly cooled glasses undergo more frequent and larger particle rearrangements than slowly cooled glasses. We find that the ratio of the shear to bulk moduli decreases with increasing cooling rate, which suggests that more rapidly cooled glasses are more ductile than slowly cooled samples. In addition, we characterized the degree of reversibility of particle motion during cyclic shear. We find that irreversible particle motion occurs even in the putative linear regime of stress versus strain. However, slowly cooled glasses, which undergo smaller rearrangements, are more reversible under cyclic shear than rapidly cooled glasses. Thus, we show that more ductile glasses are also less reversible.

cond-mat.soft↗

arXiv2016

Predicting Bulk Metallic Glass Forming Ability with the Thermodynamic Density of Competing Crystalline States

Despite two decades of studies, the formation of metallic glasses, very promising systems for industrial applications, still remains mostly unexplained. This lack of knowledge hinders the search for new systems, still performed with combinatorial trial and error. In the past, it was speculated that some sort of "confusion" during crystallization could play a key role during their formation. In this article, we propose a heuristic descriptor quantifying such confusion. It is based on the "thermodynamic density of competing crystalline states", parameterized from high-throughput ab-initio calculations. The existence of highly enthalpy-degenerate but geometrically-different phases frustrates the crystallization process and promotes glass formation. Two test beds are considered. A good and a bad glass-former, CuZr and NiZr, are experimentally characterized with high-throughput synthesis. The experimental results corroborate the capability of the heuristic descriptor in predicting glass forming ability through the compositional space. Our analysis is expected to deepen the understanding of the underlying mechanisms and to accelerate the discovery of novel metallic glasses.

cond-mat.mtrl-sci↗

arXiv2015

Beyond packing of hard spheres: The effects of core softness, non-additivity, intermediate-range repulsion, and many-body interactions on the glass-forming ability of bulk metallic glasses

When a liquid is cooled well below its melting temperature at a rate that exceeds the critical cooling rate $R_c$, the crystalline state is bypassed and an amorphous glassy state forms instead. $R_c$ (or the corresponding critical casting thickness $d_c$) characterizes the glass-forming ability (GFA) of each material. While silica is an excellent glass-former with small $R_c<10^{-2}$ K/s, pure metals and most alloys are poor glass-formers with large $R_c>10^{10}$ K/s. Only in the past thirty years have bulk metallic glasses (BMGs) been identified with $R_c$ approaching that for silica. Recent simulations have shown that hard-sphere models are able to identify the atomic size ratio and number fraction regime where BMGs exist with critical cooling rates more than 13 orders of magnitude smaller than those for pure metals. However, there are many other features of interatomic potentials beyond hard-core interactions. How do these other features affect the glass-forming ability of BMGs? We perform molecular dynamics simulations to determine how variations in the softness and non-additivity of the repulsive core and form of the interatomic pair potential at intermediate distances affect the GFA of binary alloys. These variations in the interatomic pair potential allow us to introduce geometric frustration and change the crystal phases that compete with glass formation. We also investigate the effect of tuning the strength of the many-body interactions from zero to the full embedded atom model on the GFA for pure metals. We then employ the full embedded atom model for binary BMGs and show that hard-core interactions play the dominant role in setting the GFA of alloys, while other features of the interatomic potential only change the GFA by one to two orders of magnitude.

cond-mat.mtrl-sci↗

arXiv2015

Shear accelerated crystallization in a supercooled atomic liquid

A bulk metallic glass forming alloy is subjected to shear flow in its supercooled state by compression of a short rod to produce a flat disc. The resulting material exhibits enhanced crystallization kinetics during isothermal annealing as reflected in the decrease of the crystallization time relative to the non-deformed case. The transition from quiescent to shear-accelerated crystallization is linked to strain accumulated during shear flow above a critical shear rate $\dotγ_c\approx 0.3$ s$^{-1}$ which corresponds to Péclet number, $Pe\sim\mathcal{O}(1)$. The observation of shear accelerated crystallization in an atomic system at modest shear rates is uncommon. It is made possible here by the substantial viscosity of the supercooled liquid which increases strongly with temperature in the approach to the glass transition. We may therefore anticipate the encounter of non-trivial shear-related effects during thermoplastic deformation of similar systems.

cond-mat.mtrl-sci↗