arXiv subjects

David A. Muller

Publications and source records attributed to David A. Muller.

At least 37 records · Page 2Linked to original sources

arXiv2026

Mind the Gap -- Imaging Buried Interfaces in Twisted Oxide Moirés

The ability to tune electronic structure in twisted stacks of two-dimensional (2D) materials has motivated the exploration of similar moiré physics with twisted oxide membranes. Due to the intrinsic three-dimensional nature of bonding in many oxides, achieving atomic-level coupling is significantly more challenging than with van der Waals materials. Although clean interfaces with atomic-level proximity have been demonstrated in ceramic bicrystals using high-temperature and high-pressure processing to facilitate atomic diffusion that flattens rough interfaces, such conditions are not readily accessible when bonding oxide membranes. This study shows how topographic mismatch due to surface roughness of the membranes can restrict atomic-scale proximity at the interface to isolated patches even after contaminants and amorphous interlayers are eliminated. In interfaces between 2D materials and oxide membranes the reduced ability of the 2D material to conform to the membrane's step-terrace topography also limits atomic-scale contact. When imaging stacked membranes in projection, we find conventional through-focal imaging to be relatively insensitive to the buried interface, whereas electron ptychography detects structural variations on the order of a nanometer. These findings highlight interface roughness as a key challenge for the field of oxide twistronics and emphasize the need for reliable characterization methods, both in cross-section and projection.

cond-mat.mtrl-sci↗

arXiv2026

Above Room Temperature Ferroelectricity in Epitaxially Strained KTaO3

Epitaxial strain is a powerful means to engineer emergent phenomena in thin films and heterostructures. Here, we demonstrate that KTaO3, a cubic perovskite in bulk form, can be epitaxially strained into a highly tunable ferroelectric. KTaO3 films grown commensurate to SrTiO3 (001) substrates experience an in-plane strain of -2.1 % that transforms the cubic structure into a tetragonal polar phase with transition temperature of 475 K, consistent with our thermodynamic calculations. We show that the Curie temperature and the spontaneous electric polarization can be system- atically controlled with epitaxial strain. Scanning transmission electron microscopy reveals cooperative polar displacements of the potassium columns with respect to the neighboring tantalum columns at room temperature. Optical second-harmonic generation results are described by a tetragonal polar point group (4mm), indicating the emergence of a global polar ground state. We observe a ferroelectric hysteresis response, using metal-insulator-metal capacitor test structures. The results demon- strate a robust intrinsic ferroelectric state in epitaxially strained KTaO3 thin films.

cond-mat.mtrl-sci↗

arXiv2025

Effect of substrate miscut angle on critical thickness, structural and electronic properties of MBE-grown NbN films on c-plane sapphire

We report the structural and electronic properties of niobium nitride (NbN) thin films grown by molecular beam epitaxy on c-plane sapphire with miscut angles of $0.5^\text{o}$, $2^\text{o}$, $4^\text{o}$, and $10^\text{o}$ towards m-axis. X-ray diffraction (XRD) scans reveal that the full width at half maximum of the rocking curves around the 1 1 1 reflection of these NbN films decreases with increasing miscut. Starting from 76 arcsecs on $0.5^\text{o}$ miscut, the FWHM reduces to almost 20 arcsecs on $10^\text{o}$ miscut sapphire indicating improved structural quality. Scanning transmission electron microscopy (STEM) images indicate that NbN on c-sapphire has around 10 nm critical thickness, irrespective of the substrate miscut, above which it turns columnar. The improved structural property is correlated with a marginal increment in superconducting transition temperature $T_\text{c}$ from 12.1 K for NbN on $0.5^\text{o}$ miscut sapphire to 12.5 K for NbN on $10^\text{o}$ miscut sapphire.

cond-mat.supr-con↗

arXiv2025

All-nitride superconducting qubits based on atomic layer deposition

The development of large-scale quantum processors benefits from superconducting qubits that can operate at elevated temperatures and be fabricated with scalable, foundry-compatible processes. Atomic layer deposition (ALD) is increasingly being adopted as an industrial standard for thin-film growth, particularly in applications requiring precise control over layer thickness and composition. Here, we report superconducting qubits based on NbN/AlN/NbN trilayers deposited entirely by ALD. By varying the number of ALD cycles used to form the AlN barrier, we achieve Josephson tunneling through barriers of different thicknesses, with critical current density spanning seven orders of magnitude, demonstrating the uniformity and versatility of the process. Owing to the high critical temperature of NbN, transmon qubits based on these all-nitride trilayers exhibit microsecond-scale relaxation times, even at temperatures above 300 mK. These results establish ALD as a viable low-temperature deposition technique for superconducting quantum circuits and position all-nitride ALD qubits as a promising platform for operation at elevated temperatures.

quant-ph↗

arXiv2025

Disorder-broadened topological Hall phase and anomalous Hall scaling in FeGe

Magnetic skyrmions are topologically protected spin textures that are promising candidates for low-power spintronic memory and logic devices. Realizing skyrmion-based devices requires an understanding of how structural disorder affects their stability and transport properties. This study uses Ne$^{+}$ ion irradiation at fluences from $10^{11}$ to $10^{14}$ ions-cm$^{-2}$ to systematically vary defect densities in 80 nm epitaxial FeGe films and quantify the resulting modifications to magnetic phase boundaries and electronic scattering. Temperature- and field-dependent Hall measurements reveal that increasing disorder progressively extends the topological Hall signal from a narrow window near 200K in pristine films down to 4K at the highest fluence, with peak amplitude more than doubling. Simultaneously, the anomalous Hall effect transitions from quadratic Berry curvature scaling to linear skew scattering behavior, with the skew coefficient increasing threefold. These results establish quantitative correlations between defect concentration, skyrmion phase space, and transport mechanisms in a chiral magnet. It demonstrates that ion-beam modification provides systematic control over both topological texture stability and electrical detectability.

cond-mat.mtrl-sci↗

arXiv2025

Melting point depression of charge density wave in 1T-TiSe$_2$ due to size effects

Classical nucleation theory predicts size-dependent nucleation and melting due to surface and confinement effects at the nanoscale. In correlated electronic states, observation of size-dependent nucleation and melting is rarely reported, likely due to the extremely small length scales necessary to observe such effects for electronic states. Here, using 1T-TiSe$_2$ nanoflakes as a prototypical two-dimensional (2D) charge density wave (CDW) system, we perform in-situ cryogenic electron microscopy with temperature down to 20 K and observe size-dependent nucleation and melting of CDWs. Specifically, we observe a melting point depression of CDW for 1T-TiSe$_2$ flakes with lateral sizes less than 100 nm. By fitting experimental data to a Ginzburg-Landau model, we estimate a zero-temperature correlation length of 10--50 nm, which matches the reported CDW domain size for 1T-TiSe$_2$. As the flake size approaches the correlation length, the divergence of the CDW correlation length near the transition is cut off by the finite flake size, limiting long-range order and thereby lowering the transition temperature. For very small flakes whose size is close to the correlation length, we also observe absence of CDWs, as predicted by the model. We thus show that an electronic phase transition follows classical nucleation theory.

cond-mat.mtrl-sci↗

arXiv2025

Detective quantum efficiency based comparison of HRTEM and ptychography phase imaging

High-resolution transmission electron microscopy (HRTEM) is an important method for imaging beam sensitive materials often under cryo conditions. Electron ptychography in the scanning transmission electron microscope (STEM) has been shown to reconstruct low-noise phase data at a reduced fluence for such materials. This raises the question of whether ptychography or HRTEM provides a more fluence-efficient imaging technique. Even though the transfer function is a common metric for evaluating the performance of an imaging method, it only describes the signal transfer with respect to spatial frequency, irrespective of the noise transfer. It can also not be well defined for methods, such as ptychography, that use an algorithm to form the final image. Here we apply the concept of detective quantum efficiency (DQE) to electron microscopy as a fluence independent and sample independent measure of technique performance. We find that, for a weak-phase object, ptychography can never reach the efficiency of a perfect Zernike phase imaging microscope but that ptychography is more robust to partial coherence.

cond-mat.mtrl-sci↗

arXiv2025

Cepstral Strain Mapping for Small Pixel-Count Detectors

With the decreasing sizes of integrated-circuit components, the semiconductor industry is in growing need of high-throughput strain mapping techniques that offer high precision and spatial resolution, with desired industry goals of 0.01-0.1% and 1 nm respectively. As the fundamental limitation on the measurement precision is set by the Poisson noise, pixel array detectors with high saturation current, high dynamic range and fast readout are ideally suited for this purpose. However, due to the limited pixel count on these detectors, they do not work well with traditional strain mapping algorithms that were optimized to work on datasets with a large pixel count. Here, we evaluate the cepstral transform that was designed to address this problem, with the precision determined by the convergence, collection angles and dose while remaining insensitive to the pixel count. We test the performance of our method on silicon wedges and Si-SiGe multilayers, and using datasets collected at different conditions, we show how the measured strain precision scales as a function of dose, aperture size and sample thickness. Using precession gives a further improvement in precision by about 1.5-2x, whereas energy filtering does not have a significant impact on the cepstral method for device-relevant sample thickness ranges.

physics.ins-det↗

arXiv2025

Superconductivity and normal-state transport in compressively strained La$_2$PrNi$_2$O$_7$ thin films

The discovery of superconductivity under high pressure in Ruddlesden-Popper phases of bulk nickelates has sparked great interest in stabilizing ambient pressure superconductivity in thin-film form using epitaxial strain. Recently, signs of superconductivity have been observed in compressively strained bilayer nickelate thin films with an onset temperature exceeding 40 K, albeit with broad and two-step-like transitions. Here, we report intrinsic superconductivity and normal-state transport properties in compressively strained La$_2$PrNi$_2$O$_7$ thin films, achieved through a combination of isovalent Pr substitution, growth optimization, and precision ozone annealing. The superconducting onset occurs above 48 K, with zero resistance reached above 30 K, and the critical current density at 1.4 K is 100-fold larger than previous reports. The normal-state resistivity exhibits quadratic temperature dependence indicative of Fermi liquid behaviour, and other phenomenological similarities to transport in overdoped cuprates suggest parallels in their emergent properties.

cond-mat.supr-con↗

arXiv2025

Physically-Based Inverse Rendering Framework for PET Image Reconstruction

Differentiable rendering has been widely adopted in computer graphics as a powerful approach to inverse problems, enabling efficient gradient-based optimization by differentiating the image formation process with respect to millions of scene parameters. Inspired by this paradigm, we propose a physically-based inverse rendering (IR) framework, the first ever platform for PET image reconstruction using Dr.Jit, for PET image reconstruction. Our method integrates Monte Carlo sampling with an analytical projector in the forward rendering process to accurately model photon transport and physical process in the PET system. The emission image is iteratively optimized using voxel-wise gradients obtained via automatic differentiation, eliminating the need for manually derived update equations. The proposed framework was evaluated using both phantom studies and clinical brain PET data acquired from a Siemens Biograph mCT scanner. Implementing the Maximum Likelihood Expectation Maximization (MLEM) algorithm across both the CASToR toolkit and our IR framework, the IR reconstruction achieved a higher signal-to-noise ratio (SNR) and improved image quality compared to CASToR reconstructions. In clinical evaluation compared with the Siemens Biograph mCT platform, the IR reconstruction yielded higher hippocampal standardized uptake value ratios (SUVR) and gray-to-white matter ratios (GWR), indicating enhanced tissue contrast and the potential for more accurate tau localization and Braak staging in Alzheimer's disease assessment. The proposed IR framework offers a physically interpretable and extensible platform for high-fidelity PET image reconstruction, demonstrating strong performance in both phantom and real-world scenarios.

physics.med-ph↗

arXiv2025

Electron Ptychography Images Hydrogen Atom Superlattices and 3D Inhomogeneities in Palladium Hydride Nanoparticles

When hydrogen atoms occupy interstitial sites in metal lattices, they form metal hydrides (MHx), whose structural and electronic properties can differ significantly from the host metals. Owing to the small size of hydrogen atom and its unique interactions with the host metal, MHx is of broad interest in both fundamental science and technological applications. Determining where the hydrogen is located within the MHx, and whether it orders on the partially occupied interstitial sites is crucial for predicting and understanding the resultant physical and electronic properties of the hydride. Directly imaging hydrogen within a host material remains a major challenge due to its weak interaction with X-rays and electrons in conventional imaging techniques. Here, we employ electron ptychography, a scanning transmission electron microscopy technique, to image the three-dimensional (3D) distribution of H atoms in Palladium hydrides (PdHx) nanocubes, one of the most studied and industrially relevant MHx materials. We observe an unexpected one-dimensional superlattice ordering of hydrogen within the PdHx nanocubes and 3D hydrogen clustering in localized regions within PdHx nanocubes, revealing spatial heterogeneity in metal hydride nanoparticles previously inaccessible by other methods.

cond-mat.mtrl-sci↗

arXiv2025

Low barrier ZrO$_x$-based Josephson junctions

The Josephson junction is a crucial element in superconducting devices, and niobium is a promising candidate for the superconducting material due to its large energy gap relative to aluminum. AlO$_x$ has long been regarded as the highest quality oxide tunnel barrier and is often used in niobium-based junctions. Here we propose ZrO$_x$ as an alternative tunnel barrier material for Nb electrodes. We theoretically estimate that zirconium oxide has excellent oxygen retention properties and experimentally verify that there is no significant oxygen diffusion leading to NbO$_x$ formation in the adjacent Nb electrode. We develop a top-down, subtractive fabrication process for Nb/Zr-ZrO$_x$/Nb Josephson junctions, which enables scalability and large-scale production of superconducting electronics. Using cross sectional scanning transmission electron microscopy, we experimentally find that depending on the Zr thickness, ZrO$_x$ tunnel barriers can be fully crystalline with chemically abrupt interfaces with niobium. Further analysis using electron energy loss spectroscopy reveals that ZrO$_x$ corresponds to tetragonal ZrO$_2$. Room temperature characterization of fabricated junctions using Simmons' model shows that ZrO$_2$ exhibits a low tunnel barrier height, which is promising in merged-element transmon applications. Low temperature transport measurements reveal sub-gap structure, while the low-voltage sub-gap resistance remains in the megaohm range.

cond-mat.supr-con↗

arXiv2025

Improving Multislice Electron Ptychography with a Generative Prior

Multislice electron ptychography (MEP) is an inverse imaging technique that computationally reconstructs the highest-resolution images of atomic crystal structures from diffraction patterns. Available algorithms often solve this inverse problem iteratively but are both time consuming and produce suboptimal solutions due to their ill-posed nature. We develop MEP-Diffusion, a diffusion model trained on a large database of crystal structures specifically for MEP to augment existing iterative solvers. MEP-Diffusion is easily integrated as a generative prior into existing reconstruction methods via Diffusion Posterior Sampling (DPS). We find that this hybrid approach greatly enhances the quality of the reconstructed 3D volumes, achieving a 90.50% improvement in SSIM over existing methods.

eess.IV↗

arXiv2025

PtyRAD: A High-performance and Flexible Ptychographic Reconstruction Framework with Automatic Differentiation

Electron ptychography has recently achieved unprecedented resolution, offering valuable insights across diverse material systems, including in three dimensions. However, high-quality ptychographic reconstruction is computationally expensive and time consuming, requiring a significant amount of manually tuning even for experts. Additionally, essential tools for ptychographic analysis are often scattered across multiple software packages, with some advanced features available only in costly commercial software like MATLAB. To address these challenges, we introduce PtyRAD, an open-source software framework offers a comprehensive, flexible, and computationally efficient solution for electron ptychography. PtyRAD provides seamless optimization of multiple parameters--such as sample thickness, local tilts, probe positions, and mixed probe and object modes--using gradient-based methods with automatic differentiation (AD). By utilizing PyTorch's highly optimized tensor operations, PtyRAD achieves up to a 17x speedup in reconstruction time compared to existing packages without compromising image quality. In addition, we propose a real-space depth regularization, which avoids wrap-around artifacts and can be useful for twisted two-dimensional (2D) material datasets and vertical heterostructures. Moreover, PtyRAD integrates a Bayesian optimization workflow that streamlines hyperparameter selection. We hope the open-source nature of PtyRAD will foster reproducibility and community-driven development for future advances in ptychographic imaging.

cond-mat.mtrl-sci↗

arXiv2025

3D Atomic-Scale Metrology of Strain Relaxation and Roughness in Gate-All-Around (GAA) Transistors via Electron Ptychography

To improve transistor density and electronic performance, next-generation semiconductor devices are adopting three-dimensional architectures and feature sizes down to the few-nm regime, which require atomic-scale metrology to identify and resolve performance-limiting fabrication challenges. X-ray methods deliver three-dimensional imaging of integrated circuits but lack the spatial resolution to characterize atomic-scale features, while conventional electron microscopy offers atomic-scale imaging but limited depth information. We demonstrate how multislice electron ptychography (MEP), a computational electron microscopy technique with sub-Ångström lateral and nanometer-scale depth resolution, enables 3D imaging of buried features in devices. By performing MEP on prototype gate-all-around transistors we uncover and quantify distortions and defects at the interface of the 3D gate oxide wrapped around the channel. We find that the silicon in the 5-nm-thick channel gradually relaxes away from the interfaces, leaving only 60% of the atoms in a bulk-like structure. Quantifying the interface roughness, which was not previously possible for such small 3D structures but strongly impacts carrier mobility, we find that the top and bottom interfaces show different atomic-scale roughness profiles, reflecting their different processing conditions. By measuring 3D interface roughness simultaneously with strain relaxation and atomic-scale defects, from a single MEP dataset, we provide direct experimental values of these performance-limiting parameters needed for modeling and early fabrication optimization.

cond-mat.mtrl-sci↗

arXiv2025

Unconventional superlattice ordering in intercalated transition metal dichalcogenide V$_{1/3}$NbS$_2$

The interplay between symmetry and topology in magnetic materials makes it possible to engineer exotic phases and technologically useful properties. A key requirement for these pursuits is achieving control over local crystallographic and magnetic structure, usually through sample morphology (such as synthesis of bulk crystals versus thin-films) and application of magnetic or electric fields. Here we show that V$_{1/3}$NbS$_2$ can be crystallized in two ordered superlattices, distinguished by the periodicity of out-of-plane magnetic intercalants. Whereas one of these structures is metallic and displays the hallmarks of altermagnetism, the other superlattice, which has not been isolated before in this family of intercalation compounds, is a semimetallic noncollinear antiferromagnet that may enable access to topologically nontrivial properties. This observation of an unconventional superlattice structure establishes a powerful route for tailoring the tremendous array of magnetic and electronic behaviors hosted in related materials.

cond-mat.mtrl-sci↗

arXiv2025

Microscopic mechanisms of flexoelectricity in oxide membranes

Modern electromechanical actuators and sensors rely on the piezoelectric effect that linearly couples strain and electric polarization. However, this effect is restricted to materials that lack inversion symmetry. In contrast, the flexoelectric effect couples strain gradients to electric polarization, and is a universal property in insulating materials of arbitrary symmetry. Flexoelectricity becomes prominent at the nanoscale from the inverse scaling of strain gradients with material dimensions. Here, we measure the strain-gradient-induced structural distortions in strontium titanate using multislice electron ptychography. This technique enables reliable picometer-scale measurements of the dominant oxygen-titanium distortions, correcting for artifacts that limited conventional imaging methods. This enables us to directly measure the sign of the net ionic contribution to the flexoelectric polarization. Guided by the experimental measurements, first-principles calculations show how the sign and magnitude of the bulk contribution to the flexoelectric coefficient in strontium titanate can be switched by tuning the strain state. Hybridization between the optical soft phonon and acoustic phonon modes drives this transition, yielding a large response and a polarity switch across the resonance. This strain-dependence might explain the sign discrepancy and orders of magnitude variation in the values of previously reported flexoelectric coefficients for strontium titanate. As the strain state of curved membranes can be tuned, our approach also suggests an approach to engineer nanoscale flexoelectric polarization using strain as a control parameter.

cond-mat.mtrl-sci↗

arXiv2025

Superconductivity in tin telluride films grown by molecular beam epitaxy

The intersection of superconductivity and ferroelectricity hosts a wide range of exotic quantum phenomena. Here, we report on the observation of superconductivity in high-quality tin telluride films grown by molecular beam epitaxy. Unintentionally doped tin telluride undergoes a ferroelectric transition at ~100 K. The critical temperature of superconductivity increases monotonically with indium concentration. The critical field of superconductivity, however, does not follow the same behavior as critical temperature with indium concentration and exhibits a carrier-density-dependent violation of the Pauli limit. The electron-phonon coupling, from the McMillan formula, exhibits a systematic enhancement with indium concentration, suggesting a potential violation of BCS weak coupling at high indium concentrations.

cond-mat.supr-con↗