Paul M Voyles

• University of Wisconsin–Madison

In recent years, Td transition metal dichalcogenides have been heavily explored for their type‐II Weyl topology, gate‐tunable superconductivity, and nontrivial edge states in the monolayer limit. Here, the Fermi surface characteristics and fundamental transport properties of similarly structured 2M‐WSe2 bulk single crystals are investigated. The me...

In alignment with the Materials Genome Initiative and as the product of a workshop sponsored by the US National Science Foundation, we define a vision for materials laboratories of the future in alloys, amorphous materials, and composite materials; chart a roadmap for realizing this vision; identify technical bottlenecks and barriers to access; and...

Tantalum films incorporated into superconducting circuits have exhibited low surface losses, resulting in long-lived qubit states. The remaining loss pathways originate in microscopic defects that manifest as two level systems (TLSs) at low temperatures. These defects limit performance, so careful attention to tantalum film structures is critical f...

One compelling vision of the future of materials discovery and design involves the use of machine learning (ML) models to predict materials properties and then rapidly find materials tailored for specific applications. However, realizing this vision requires both providing detailed uncertainty quantification (model prediction errors and domain of a...

Hexagonal $ABC$ intermetallics are predicted to have tunable ferroelectric, topological, and magnetic properties as a function of the polar buckling of $BC$ atomic planes. We report the impact of isovalent lanthanide substitution on the buckling, structural phase transitions, and electronic and magnetic properties of Gd$_x$La$_{1-x}$PtSb films grow...

One compelling vision of the future of materials discovery and design involves the use of machine learning (ML) models to predict materials properties and then rapidly find materials tailored for specific applications. However, realizing this vision requires both providing detailed uncertainty quantification (model prediction errors and domain of a...

Remote and van der Waals epitaxy are promising approaches for synthesizing single crystalline membranes for flexible electronics and discovery of new properties via extreme strain; however, a fundamental challenge is that most materials do not wet the graphene surface. We develop a cold seed approach for synthesizing smooth intermetallic films on g...

Electron counting can be performed algorithmically for monolithic active pixel sensor direct electron detectors to eliminate readout noise and Landau noise arising from the variability in the amount of deposited energy for each electron. Errors in existing counting algorithms include mistakenly counting a multielectron strike as a single electron e...

Physical vapor deposition (PVD) provides a route to prepare highly stable and anisotropic organic glasses that are utilized in multi-layer structures such as organic light-emitting devices. While previous work has demonstrated that anisotropic glasses with uniaxial symmetry can be prepared by PVD, here, we prepare biaxially aligned glasses in which...

Two-dimensional (2D) magnets exhibit unique physical properties for potential applications in spintronics. To date, most 2D ferromagnets are obtained by mechanical exfoliation of bulk materials with van der Waals interlayer interactions, and the synthesis of single- or few-layer 2D ferromagnets with strong interlayer coupling remains experimentally...

We examine the effects of Pt vacancies on the magnetotransport properties of Weyl semimetal candidate GdPtSb films, grown by molecular beam epitaxy on c-plane sapphire. Rutherford backscattering spectrometry and x-ray diffraction measurements suggest that phase-pure GdPtxSb films can accommodate up to 15% of Pt vacancies (x=0.85), which act as acce...

Bulk metallic glasses can exhibit novel material properties for engineering scale components, but the experimental discovery of new alloy compositions is time intensive and thwarts the rate of discovery. This study presents an experimental, high-throughput methodology to increase the speed of discovery for potential bulk metallic glass alloys. A we...

We use a random forest model to predict the critical cooling rate (RC) for glass formation of various alloys from features of their constituent elements. The random forest model was trained on a database that integrates multiple sources of direct and indirect RC data for metallic glasses to expand the directly measured RC database of less than 100...

X-ray scattering has been used to characterize the columnar packing and the π stacking in a glass-forming discotic liquid crystal. In the equilibrium liquid state, the intensities of the scattering peaks for π stacking and columnar packing are proportional to each other, indicating concurrent development of the two orders. Upon cooling into the gla...

We examine the effects of Pt vacancies on the magnetotransport properties of Weyl semimetal candidate GdPtSb films, grown by molecular beam epitaxy on c-plane sapphire. Rutherford backscattering spectrometry (RBS) and x-ray diffraction measurements suggest that phase pure GdPt$_{x}$Sb films can accommodate up to $15\%$ Pt vacancies ($x=0.85$), whic...

Physical vapor deposition can be used to prepare highly stable organic glass systems where the molecules show orientational and translational ordering at the nanoscale. We have used low-dose four-dimensional scanning transmission electron microscopy (4D STEM), enabled by a fast direct electron detector, to map columnar order in glassy samples of a...

Physical vapor deposition can be used to prepare highly stable organic glass systems where the molecules show orientational and translational ordering at the nanoscale. We have used low-dose four-dimensional scanning transmission electron microscopy (4D STEM), enabled by a fast direct electron detector, to map columnar order in glassy samples of a...

The high density of aluminum nanocrystals (>10 ²¹ m ⁻³ ) that develop during the primary crystallization in Al-based metallic glasses indicates a high nucleation rate (∼10 ¹⁸ m ⁻³ s ⁻¹ ). Several studies have been advanced to account for the primary crystallization behavior, but none have been developed to completely describe the reaction kinetics....

Primary crystallization in high Al-content metallic glasses is driven by nanometer-diameter regions with internal structure similar to fcc Al. Comparison of fluctuation electron microscopy (FEM) data to FEM simulations of fcc Al clusters dispersed in a dense-random packed matrix is used to extract the diameter and volume fraction of the ordered reg...

The information content of atomic-resolution scanning transmission electron microscopy (STEM) images can often be reduced to a handful of parameters describing each atomic column, chief among which is the column position. Neural networks (NNs) are high performance, computationally efficient methods to automatically locate atomic columns in images,...

Short-timescale atomic rearrangements are fundamental to the kinetics of glasses and frequently dominated by one atom moving significantly (a rearrangement), while others relax only modestly. The rates and directions of such rearrangements (or hops) are dominated by the distributions of activation barriers ( E act ) for rearrangement for a single a...

Short-timescale atomic rearrangements are fundamental to the kinetics of glasses and frequently dominated by one atom moving significantly (a rearrangement), while others relax only modestly. The rates and directions of such rearrangements (or hops) are dominated by the distributions of activation barriers (Eact) for rearrangement for a single atom...

Densely spaced four-dimensional scanning transmission electron microscopy (4D STEM) analyzed using correlation symmetry coefficients enables large area mapping of approximate rotational symmetries in amorphous materials. Here, we report the effects of Poisson noise, limited electron counts, probe coherence, reciprocal space sampling, and the probe-...

The isothermal and cyclic oxidation behavior of Mo-6Si-12B-(1, 2, 4, 8)Al samples was investigated from 800 to 1300℃. With increasing Al content, the isothermal oxidation resistance is enhanced and the pesting behavior is suppressed at 800℃. The Mo-6Si-12B-4Al alloy with an oxide layer of both an alumino-borosilicate glasses and mullite has the bes...

The information content of atomic resolution scanning transmission electron microscopy (STEM) images can often be reduced to a handful of parameters describing each atomic column, chief amongst which is the column position. Neural networks (NNs) are a high performance, computationally efficient method to automatically locate atomic columns in image...

Scanning transmission electron microscopy (STEM) has emerged as a uniquely powerful tool for structural and functional imaging of materials on the atomic level. Driven by advances in aberration correction, STEM now allows the routine imaging of structures with single-digit picometre-level precision for localization of atomic units. This Primer focu...

Hydrogenated amorphous carbon coatings improve mechanical performance characteristics on a variety of substrates, resulting in widespread industry applications requiring a combination of high hardness, low coefficient of friction, wear resistance, elasticity, and adhesion, but such a combination of properties is difficult to achieve. We investigate...

The combination of ferromagnetism and semiconducting behavior offers an avenue for realizing novel spintronics and spin-enhanced thermoelectrics. Here we demonstrate the synthesis of doped and nanocomposite half-Heusler Fe1+xVSb films by molecular beam epitaxy. For dilute excess Fe (x<0.1), we observe a decrease in the Hall electron concentration a...

We have developed models of metallic alloy glass forming ability based on newly computationally accessible features obtained from molecular dynamics simulations. Since the discovery of metallic glasses, there have been efforts to predict glass forming ability (GFA) for new alloys. Effective evaluations of GFA have been obtained but generally relied...

Recent machine learning models for band gap prediction that encode the structure information explicitly to the model feature set significantly improve the model accuracy compared to both traditional machine learning and non-graph-based deep learning methods. The ongoing rapid growth of open-access band gap databases can benefit such model construct...

Angular symmetry in diffraction reflects rotational symmetry in the sample. We introduce the angular symmetry coefficient as a method to extract local symmetry information from electron nanodiffraction patterns of amorphous materials. Symmetry coefficients are the average of the angular autocorrelation function at the characteristic angles of a par...

The bulk and surface dynamics of Cu50Zr50 metallic glass were studied using classical molecular dynamics (MD) simulations. As the alloy undergoes cooling, it passes through liquid, supercooled, and glassy states. While bulk dynamics showed a marked slowing down prior to glass formation, with increasing activation energy, the slowdown in surface dyn...

We have developed models of metallic alloy glass forming ability based on newly computationally accessible features obtained from molecular dynamics simulations. In this work we showed that it is possible to increase the predictive value of GFA models by using input features obtained from molecular dynamics simulations. Such features require only r...

The enhancement of surface diffusion (DS) over the bulk (DV) in metallic glasses (MGs) is well documented and likely to strongly influence the properties of glasses grown by vapor deposition. Here, we use classical molecular dynamics simulations to identify different factors influencing the enhancement of surface diffusion in MGs. MGs have a simple...

Author Various combinations of characteristic temperatures, such as the glass transition temperature, liquidus temperature, and crystallization temperature, have been proposed as predictions of the glass forming ability of metal alloys. We have used statistical approaches from machine learning to systematically explore a wide range of possible char...

Various combinations of characteristic temperatures, such as the glass transition temperature, liquidus temperature, and crystallization temperature, have been proposed as predictions of the glass forming ability of metal alloys. We have used statistical approaches from machine learning to systematically explore a wide range of possible characteris...

The combination of ferromagnetism and semiconducting behavior offers an avenue for realizing novel spintronics and spin-enhanced thermoelectrics. Here we demonstrate the synthesis of doped and nanocomposite half Heusler Fe$_{1+x}$VSb films by molecular beam epitaxy. For dilute excess Fe ($x < 0.1$), we observe a decrease in the Hall electron concen...

Single-crystalline membranes of functional materials enable the tuning of properties via extreme strain states; however, conventional routes for producing membranes require the use of sacrificial layers and chemical etchants, which can both damage the membrane and limit the ability to make them ultrathin. Here we demonstrate the epitaxial growth of...

The enhancement of surface diffusion (DS) over the bulk (DV) in metallic glasses (MGs) is well documented and likely to strongly influence the properties of glasses grown by vapor deposition. Here, we use classical molecular dynamics (MD) simulations to identify different factors influencing the enhancement of surface diffusion in MGs. MGs have a s...

Zr65Cu27.5Al7.5 metallic glass thin films with widely varying kinetic stability as a function of deposition rate were synthesized by single-target direct current magnetron sputtering. Fluctuation electron microscopy and angular correlations in coherent electron nanodiffraction show that glasses with increased stability have increased nanoscale stru...

The bulk and surface dynamics of Cu50Zr50 metallic glass were studied using classical molecular dynamics (MD) simulations. As the alloy undergoes cooling, it passes through liquid, supercooled, and glassy states. While bulk dynamics showed a marked slowing down prior to glass formation, with increasing activation energy, the slowdown in surface dyn...

Tensor singular value decomposition (SVD) is a method to find a low-dimensional representation of data with meaningful structure in three or more dimensions. Tensor SVD has been applied to denoise atomic-resolution 4D scanning transmission electron microscopy (4D STEM) data. On data simulated from a SrTiO3 [100] perfect crystal and a Si [110] edge...

Achieving sub-picometer precision measurements of atomic column positions in high-resolution scanning transmission electron microscope images using nonrigid registration (NRR) and averaging of image series requires careful optimization of experimental conditions and the parameters of the registration algorithm. On experimental data from SrTiO3 [100...

Using curves to make twists The growth of layered materials on flat substrates usually occurs in stacked layers, although defects or a lattice mismatch can induce strains that distort the shape of subsequent layers. However, these effects are usually small and can be uncontrolled. Zhao et al. now demonstrate the possibility of synthesizing multilay...

Radiation-induced segregation is well known in metals, but has been rarely studied in ceramics. We discover that radiation can induce notable segregation of one of the constituent elements to grain boundaries in a ceramic, despite the fact that the ceramic forms a line compound and therefore has a strong thermodynamic driving force to resist off-st...

Denoising Atomic Resolution Hyperspectral Data with Tensor Singular Value Decomposition - Chenyu Zhang, Rungang Han, Anru Zhang, Paul Voyles

Structural Determination in Metallic Glasses from Correlations in 4D STEM Datasets - Carter Francis, Debaditya Chatterjee, Sachin Muley, Paul Voyles

“Crystallography” of an Amorphous Material Using Electron Nanodiffraction - Carter Francis, Debaditya Chatterjee, Sachin Muley, Paul Voyles

Electron Correlation Microscopy Measurements of Metallic Glass Surface Dynamics - Debaditya Chatterjee, Paul Voyles

4D Scanning Transmission Electron Microscopy of a Twisted WS2 Multilayer Structure - Chenyu Zhang, Yuzhou Zhao, Song Jin, Paul Voyles

The electronic, magnetic, thermoelectric, and topological properties of Heusler compounds (composition XYZ or X2YZ) are highly sensitive to stoichiometry and defects. Here we establish the existence and experimentally map the bounds of a semi-adsorption-controlled growth window for semiconducting half-Heusler FeVSb films, grown by molecular beam ep...

Single-crystalline membranes of functional materials enable the tuning of properties via extreme strain states; however, conventional routes for producing membranes require the use of sacrificial layers and chemical etchants, which can both damage and limit the ability to make membranes ultrathin. Here we demonstrate the epitaxial growth of cubic a...

Achieving sub-picometer precision measurements of atomic column positions in high-resolution scanning transmission electron microscope images using non-rigid registration (NRR) and averaging of image series requires careful optimization of experimental conditions and the parameters of the registration algorithm. On experimental data from SrTiO 3 [1...

The emergence of memristive behavior in amorphous–crystalline 2D oxide heterostructures, which are synthesized by atomic layer deposition (ALD) of a few‐nanometer amorphous Al2O3 layers onto atomically thin single‐crystalline ZnO nanosheets, is demonstrated. The conduction mechanism is identified based on classic oxygen vacancy conductive channels....

The electronic, magnetic, thermoelectric, and topological properties of Heusler compounds (composition $XYZ$ or $X_2 YZ$) are highly sensitive to stoichiometry and defects. Here we establish the existence and experimentally map the bounds of a \textit{semi} adsorption-controlled growth window for semiconducting half Heusler FeVSb films, grown by mo...

A major challenge for ferroelectric devices is the depolarization field, which competes with and often destroys long-range polar order in the limit of ultrathin films. Recent theoretical predictions suggest a new class of materials, termed hyperferroelectics, that should be robust against the depolarization field and enable ferroelectricity down to...

A major challenge for ferroelectric devices is the depolarization field, which competes with and often destroys long-range polar order in the limit of ultrathin films. Recent theoretical predictions suggest a new class of materials, termed hyperferroelectics, that should be robust against the depolarization field and enable ferroelectricity down to...

Polar metals are an intriguing class of materials that simultaneously host free carriers and polar structural distortions. Despite the name “polar metal,” however, most well-studied polar metals are poor electrical conductors. Here, we demonstrate the molecular beam epitaxial growth of LaPtSb and LaAuGe, two polar metal compounds whose electrical r...

Two types of convolutional neural network (CNN) models, a discrete classification network and a continuous regression network, were trained to determine local sample thickness from convergent beam diffraction (CBED) patterns of SrTiO3 collected in a scanning transmission electron microscope (STEM) at atomic column resolution. Acquisition of atomic...

Room-temperature ferromagnetism in two dimensional oxide materials is an intriguing phenomenon for spintronic applications. Here, we report a significantly enhanced room-temperature ferromagnetism observed from ultrathin cerium oxide nanosheets hybridized with organic surfactant molecules. The hybrid nanosheets were synthesized by ionic layer epita...

Polar metals are an intriguing class of materials that simultaneously host free carriers and polar structural distortions. Despite the name "polar metal," however, most well-studied polar metals are poor electrical conductors. Here, we demonstrate the molecular beam epitaxial (MBE) growth of LaPtSb and LaAuGe, two polar metal compounds whose electr...

Controllable synthesis of 2D monocrystalline oxides nanomaterials beyond van der Waals solids is intriguing but very challenging. Inspired by the biomineralization processes that commonly implement organic templates with both positive and negative charges for regulating the crystal nucleation and growth, we adapted mix-charges amphiphilic monolayer...

Polyamorphs are often observed in amorphous matters, and a representative example is the reentrant glass transition in colloid systems. For metallic amorphous alloys, however, the cases reported so far are limited to metallic glasses (MGs) that undergo electronic transitions under gigapascal applied pressure, or the presence of two liquids at the s...

Atomic Resolution Convergent Beam Electron Diffraction Analysis Using Convolutional Neural Networks - Volume 25 Supplement - Chenyu Zhang, Jie Feng, Luis Rangel DaCosta, Paul M. Voyles

Effectively Synchronizing 4D-STEM Detectors with Probe Movement - Volume 25 Supplement - Benjamin Bammes, Chenyu Zhang, Robert Bilhorn, Paul M. Voyles

Electron Correlation Microscopy for Studying Fluctuating Systems In Situ - Volume 25 Supplement - Debaditya Chatterjee, Pei Zhang, Paul M. Voyles

Proton irradiation induced Nb redistribution in Zr-xNb alloys (x = 0.4, 0.5, 1.0 wt%) has been investigated using scanning transmission electron microscopy/energy dispersive X-ray spectroscopy (STEM/EDS). Zr-xNb alloys are mainly composed of Zr matrix, native Zr–Nb–Fe phases, and β-Nb precipitates. After 2 MeV proton irradiation at 350 °C, a decrea...

The structural motifs of a Zr50Cu45Al5 metallic glass were learned from atomistic models using a new structure analysis method called motif extraction that employs point-pattern matching and machine learning clustering techniques. The motifs are the nearest-neighbor building blocks of the glass and reveal a well-defined hierarchy of structures as a...

Realization of sub‐10 nm spin‐based logic and memory devices relies on the development of magnetic materials with perpendicular magnetic anisotropy that can provide low switching current and large thermal stability simultaneously. In this work, the authors report on one promising candidate, Fe16N2, a heavy‐metal‐free, non‐interface perpendicular ma...