arXiv subjects

David A. Muller

Publications and source records attributed to David A. Muller.

At least 55 records · Page 3Linked to original sources

arXiv2025

Improper Ferroelectricity at the Monolayer Limit

Ultrathin ferroelectric films with out-of-plane polarization and high Curie temperatures are key to miniaturizing electronic devices. Most ferroelectrics employed in devices are proper ferroelectrics, where spontaneous polarization is the primary order parameter. Unfortunately, the Curie temperature of proper ferroelectrics is drastically reduced as the ferroelectric becomes thin; nearly all proper ferroelectrics need to be thicker than several unit cells. The absence of an ultrathin limit has been predicted, but not verified for improper ferroelectrics. These are ferroelectrics where the polarization emerges secondary to the primary order parameter, such as a structural distortion. Here we report improper ferroelectricity with an undiminished Curie temperature in a 0.75-unit-cell-thick hexagonal LuFeO3 (h-LuFeO3) film grown on a SrCo2Ru4O11 bottom electrode with an atomically engineered monolayer bridging layer. Our results demonstrate the absence of a critical thickness for improper ferroelectricity and provide a methodology for creating ultrathin improper ferroelectrics by stabilizing their primary order parameters.

cond-mat.mtrl-sci↗

arXiv2025

Bright hybrid excitons in molecularly tunable bilayer crystals

Bilayer crystals, built by stacking crystalline monolayers, generate interlayer potentials that govern excitonic phenomena but are constrained by fixed covalent lattices and orientations. Replacing one layer with an atomically thin molecular crystal overcomes this limitation, as diverse functional groups enable tunable molecular lattices and interlayer potentials, tailoring a wide range of excitonic properties. Here, we report hybrid excitons in four-atom-thick hybrid bilayer crystals (HBCs), directly synthesized with single-crystalline perylene diimide (PDI) molecular crystal atop WS2 monolayers. These excitons arise from a hybridized bilayer band structure, revealed by lattice-scale first-principles calculations, inheriting properties from both monolayers. They exhibit bright photoluminescence with near-unity polarization above and below the WS2 bandgap, along with spectral signatures of exciton delocalization, supported by theory, while their energies and intensities are tuned by modifying the HBC composition by synthesis. Our work introduces a molecule-based 2D quantum materials platform for bottom-up design and control of optoelectronic properties.

cond-mat.mtrl-sci↗

arXiv2025

Violation of Pauli Limit at KTaO3(110) Interfaces

The superconducting order parameter at the KTaO3 interfaces and its dependence on interface orientation remains a subject of debate. The superconductivity at these interfaces exhibits strong resilience against in-plane magnetic field and violates Pauli limit. The interface orientation dependence of critical field and violation of Pauli limit, however, have not been investigated. To address this problem, we grew epitaxial LaMnO3/KTaO3 heterostructures using molecular beam epitaxy. We show that superconductivity is extremely robust against the in-plane magnetic field. Our results indicate that the interface orientation, despite impacting the critical temperature, does not affect the ratio of critical field to the Pauli limiting field. These results offer opportunities to engineer superconductors which are resilient against magnetic field.

cond-mat.supr-con↗

arXiv2025

Spectra-orthogonal optical anisotropy in wafer-scale molecular crystal monolayers

Controlling the spectral and polarization responses of two-dimensional (2D) crystals is vital for developing ultra-thin platforms for compact optoelectronic devices. However, independently tuning optical anisotropy and spectral response remains challenging in conventional semiconductors due to the intertwined nature of their lattice and electronic structures. Here, we report spectra-orthogonal optical anisotropy, where polarization anisotropy is tuned independently of spectral response, in wafer-scale, one-atom-thick 2D molecular crystal (2DMC) monolayers synthesized on monolayer transition metal dichalcogenide (TMD) crystals. Utilizing the concomitant spectral consistency and structural tunability of perylene derivatives, we demonstrate tunable optical polarization anisotropy in 2DMCs with similar spectral profiles, as confirmed by room-temperature scanning tunneling microscopy and cross-polarized reflectance microscopy. Additional angle-dependent analysis of the single- and polycrystalline molecular domains reveals an epitaxial relationship between the 2DMC and the TMD. Our results establish a scalable, molecule-based 2D crystalline platform for unique and tunable functionalities unattainable in covalent 2D solids.

cond-mat.mes-hall↗

arXiv2025

Quantum oscillations of holes in GaN

GaN has emerged to be a major semiconductor akin to silicon due to its revolutionary impacts in solid state lighting, critically enabled by p-type doping, and high-performance radio-frequency and power electronics. Suffering from inefficient hole doping and low hole mobility, quantum oscillations in p-type GaN have not been observed, hindering fundamental studies of valence bands and hole transport in GaN. Here, we present the first observation of quantum oscillations of holes in GaN. Shubnikov-de Haas (SdH) oscillations in hole resistivity are observed in a quantum-confined two-dimensional hole gas at a GaN/AlN interface, where polarization-induced doping overcomes thermal freeze-out, and a sharp and clean interface boosts the hole mobility enough to unmask the quantum oscillations. These holes degenerately occupy the light and heavy hole bands of GaN and have record-high mobilities of ~1900 cm2/Vs and ~400 cm2/Vs at 3K, respectively. We use magnetic fields up to 72 T to resolve SdH oscillations of holes from both valence bands to extract their respective sheet densities, quantum scattering times, and the effective masses of light holes (0.5-0.7 m0) and heavy holes (1.9 m0). SdH oscillations of heavy and light holes in GaN constitute a direct metrology of valence bands and open new venues for quantum engineering in this technologically important semiconductor. Like strained silicon transistors, strain-engineering of the valence bands of GaN is predicted to dramatically improve hole mobilities by reducing the hole effective mass, a proposal that can now be explored experimentally, particularly in a fully fabricated transistor, using quantum oscillations. Furthermore, the findings of this work suggest a blueprint to create 2D hole gases and observe quantum oscillations of holes in related wide bandgap semiconductors such as SiC and ZnO in which such techniques are not yet possible.

cond-mat.mes-hall↗

arXiv2025

Emittance Minimization for Aberration Correction II: Physics-informed Bayesian Optimization of an Electron Microscope

Aberration-corrected Scanning Transmission Electron Microscopy (STEM) has become an essential tool in understanding materials at the atomic scale. However, tuning the aberration corrector to produce a sub-Ångström probe is a complex and time-costly procedure, largely due to the difficulty of precisely measuring the optical state of the system. When measurements are both costly and noisy, Bayesian methods provide rapid and efficient optimization. To this end, we develop a Bayesian approach to fully automate the process by minimizing a new quality metric, beam emittance, which is shown to be equivalent to performing aberration correction. In part I, we derived several important properties of the beam emittance metric and trained a deep neural network to predict beam emittance growth from a single Ronchigram. Here we use this as the black box function for Bayesian Optimization and demonstrate automated tuning of simulated and real electron microscopes. We explore different surrogate functions for the Bayesian optimizer and implement a deep neural network kernel to effectively learn the interactions between different control channels without the need to explicitly measure a full set of aberration coefficients. Both simulation and experimental results show the proposed method outperforms conventional approaches by achieving a better optical state with a higher convergence rate.

physics.ins-det↗

arXiv2025

Resolving Structural Origins for Superconductivity in Strain-Engineered La$_3$Ni$_2$O$_7$ Thin Films

The discovery of high-temperature superconductivity in bulk La$_3$Ni$_2$O$_7$ under high hydrostatic pressure and, more recently, biaxial compression in epitaxial thin films has ignited significant interest in understanding the interplay between atomic and electronic structure in these compounds. Subtle changes in the nickel-oxygen bonding environment are thought to be key drivers for stabilizing superconductivity, but specific details of which bonds and which modifications are most relevant remains so far unresolved. While direct, atomic-scale structural characterization under hydrostatic pressure is beyond current experimental capabilities, static stabilization of strained La$_3$Ni$_2$O$_7$ films provides a platform well-suited to investigation with new picometer-resolution electron microscopy methods. Here, we use multislice electron ptychography to directly measure the atomic-scale structural evolution of La$_3$Ni$_2$O$_7$ thin films across a wide range of biaxial strains tuned via substrate. By resolving both the cation and oxygen sublattices, we study strain-dependent evolution of atomic bonds, providing the opportunity to isolate and disentangle the effects of specific structural motifs for stabilizing superconductivity. We identify the lifting of crystalline symmetry through modification of the nickel-oxygen octahedral distortions under compressive strain as a key structural ingredient for superconductivity. Rather than previously supposed $c$-axis compression, our results highlight the importance of in-plane biaxial compression in superconducting thin films, which suggests an alternative -- possibly cuprate-like -- understanding of the electronic structure. Identifying local regions of inhomogeneous oxygen stoichiometry and high internal strain near crystalline defects, we suggest potential pathways for improving the sharpness and temperature of the superconducting transition.

cond-mat.supr-con↗

arXiv2025

Electron ptychography reveals a ferroelectricity dominated by anion displacements

Sodium niobate, a lead-free ferroic material, hosts delicately-balanced, competing order parameters, including ferroelectric states that can be stabilized by epitaxial strain. Here, we show that the resulting macroscopic ferroelectricity exhibits an unconventional microscopic structure using multislice electron ptychography. This technique overcomes multiple scattering artifacts limiting conventional electron microscopy, enabling both lateral spatial resolution beyond the diffraction limit and recovery of three-dimensional structural information. These imaging capabilities allow us to separate the ferroelectric interior of the sample from the relaxed surface structure and identify the soft phonon mode and related structural distortions with picometer precision. Unlike conventional ferroelectric perovskites, we find that the polar distortion in this material involves minimal distortions of the cation sublattices and is instead dominated by anion displacements relative to the niobium sublattice. We establish limits on film thickness for interfacial octahedral rotation engineering and directly visualize a random octahedral rotation pattern, arising from the flat dispersion of the associated phonon mode.

cond-mat.mtrl-sci↗

arXiv2024

Emittance Minimization for Aberration Correction I: Aberration correction of an electron microscope without knowing the aberration coefficients

Precise alignment of the electron beam is critical for successful application of scanning transmission electron microscopes (STEM) to understanding materials at atomic level. Despite the success of aberration correctors, aberration correction is still a complex process. Here we approach aberration correction from the perspective of accelerator physics and show it is equivalent to minimizing the emittance growth of the beam, the span of the phase space distribution of the probe. We train a deep learning model to predict emittance growth from experimentally accessible Ronchigrams. Both simulation and experimental results show the model can capture the emittance variation with aberration coefficients accurately. We further demonstrate the model can act as a fast-executing function for the global optimization of the lens parameters. Our approach enables new ways to quickly quantify and automate aberration correction that takes advantage of the rapid measurements possible with high-speed electron cameras. In part II of the paper, we demonstrate how the emittance metric enables rapid online tuning of the aberration corrector using Bayesian optimization.

physics.ins-det↗

arXiv2024

Structural Properties and Recrystallization Effects in Ion Beam Modified B20-type FeGe Films

Disordered iron germanium (FeGe) has recently garnered interest as a testbed for a variety of magnetic phenomena as well as for use in magnetic memory and logic applications. This is partially owing to its ability to host skyrmions and antiskyrmions -- nanoscale whirlpools of magnetic moments that could serve as information carriers in spintronic devices. In particular, a tunable skyrmion-antiskyrmion system may be created through precise control of the defect landscape in B20-phase FeGe, motivating developing methods to systematically tune disorder in this material and understand the ensuing structural properties. To this end, we investigate a route for modifying magnetic properties in FeGe. Specifically, we irradiate epitaxial B20-phase FeGe films with 2.8 MeV Au$^{4+}$ ions, which creates a dispersion of amorphized regions that may preferentially host antiskyrmions at densities controlled by the irradiation fluence. To further tune the disorder landscape, we conduct a systematic electron diffraction study with in-situ annealing, demonstrating the ability to recrystallize controllable fractions of the material at temperatures ranging from approximately 150$^{\circ}$ C to 250$^{\circ}$C. Finally, we describe the crystallization kinetics using the Johnson-Mehl-Avrami-Kolmogorov model, finding that the growth of crystalline grains is consistent with diffusion-controlled one-to-two dimensional growth with a decreasing nucleation rate.

cond-mat.mtrl-sci↗

arXiv2024

Lattice-Matched Multiple Channel AlScN/GaN Heterostructures

AlScN is a new wide bandgap, high-k, ferroelectric material for RF, memory, and power applications. Successful integration of high quality AlScN with GaN in epitaxial layer stacks depends strongly on the ability to control lattice parameters and surface or interface through growth. This study investigates the molecular beam epitaxy growth and transport properties of AlScN/GaN multilayer heterostructures. Single layer Al$_{1-x}$Sc$_x$N/GaN heterostructures exhibited lattice-matched composition within $x$ = 0.09 -- 0.11 using substrate (thermocouple) growth temperatures between 330 $ ^\circ$C and 630 $ ^\circ$C. By targeting the lattice-matched Sc composition, pseudomorphic AlScN/GaN multilayer structures with ten and twenty periods were achieved, exhibiting excellent structural and interface properties as confirmed by X-ray diffraction (XRD) and scanning transmission electron microscopy (STEM). These multilayer heterostructures exhibited substantial polarization-induced net mobile charge densities of up to 8.24 $\times$ 10$^{14}$/cm$^2$ for twenty channels. The sheet density scales with the number of AlScN/GaN periods. By identifying lattice-matched growth condition and using it to generate multiple conductive channels, this work enhances our understanding of the AlScN/GaN material platform.

cond-mat.mtrl-sci↗

arXiv2024

Imaging interstitial atoms with multislice electron ptychography

Doping impurity atoms is a strategy commonly used to tune the functionality of materials including catalysts, semiconductors, and quantum emitters. The location of dopants and their interaction with surrounding atoms could significantly modulate the transport, optical, or magnetic properties of materials. However, directly imaging individual impurity atoms inside materials remains a generally unaddressed need. Here, we demonstrate how single atoms can be detected and located in three dimensions via multislice electron ptychography.Interstitial atoms in a complex garnet oxide heterostructure are resolved with a depth resolution better than 2.7 nm, together with a deep-sub-Ångstrom lateral resolution. Single-scan atomic-layer depth resolution should be possible using strongly divergent electron probe illumination. Our results provide a new approach to detecting individual atomic defects and open doors to characterize the local environments and spatial distributions that underlie a broad range of systems such as single-atom catalysts, nitrogen-vacancy centers, and other atomic-scale quantum sensors.

cond-mat.mtrl-sci↗

arXiv2024

Millimeter-scale freestanding superconducting infinite-layer nickelate membranes

Progress in the study of infinite-layer nickelates has always been highly linked to materials advances. In particular, the recent development of superconductivity via hole-doping was predicated on the controlled synthesis of Ni in a very high oxidation state, and subsequent topotactic reduction to a very low oxidation state, currently limited to epitaxial thin films. Here we demonstrate a process to combine these steps with a heterostructure which includes an epitaxial soluble buffer layer, enabling the release of freestanding membranes of (Nd,Sr)NiO2 encapsulated in SrTiO3, which serves as a protective layer. The membranes have comparable structural and electronic properties to that of optimized thin films, and range in lateral dimensions from millimeters to ~100 micron fragments, depending on the degree of strain released with respect to the initial substrate. The changes in the superconducting transition temperature associated with membrane release are quite similar to those reported for substrate and pressure variations, suggestive of a common underlying mechanism. These membranes structures should provide a versatile platform for a range of experimental studies and devices free from substrate constraints.

cond-mat.mtrl-sci↗

arXiv2023

Surface oxides, carbides, and impurities on RF superconducting Nb and Nb3Sn: A comprehensive analysis

Surface structures on radio-frequency (RF) superconductors are crucially important in determining their interaction with the RF field. Here we investigate the surface compositions, structural profiles, and valence distributions of oxides, carbides, and impurities on niobium (Nb) and niobium-tin (Nb3Sn) in situ under different processing conditions. We establish the underlying mechanisms of vacuum baking and nitrogen processing in Nb and demonstrate that carbide formation induced during high-temperature baking, regardless of gas environment, determines subsequent oxide formation upon air exposure or low-temperature baking, leading to modifications of the electron population profile. Our findings support the combined contribution of surface oxides and second-phase formation to the outcome of ultra-high vacuum baking (oxygen processing) and nitrogen processing. Also, we observe that vapor-diffused Nb3Sn contains thick metastable oxides, while electrochemically synthesized Nb3Sn only has a thin oxide layer. Our findings reveal fundamental mechanisms of baking and processing Nb and Nb3Sn surface structures for high-performance superconducting RF and quantum applications

cond-mat.mtrl-sci↗

arXiv2023

Smooth, homogeneous, high-purity Nb3Sn superconducting RF resonant cavity by seed-free electrochemical synthesis

Workbench-size particle accelerators, enabled by Nb3Sn-based superconducting radio-frequency (SRF) cavities, hold the potential of driving scientific discovery by offering a widely accessible and affordable source of high-energy electrons and X-rays. Thin-film Nb3Sn RF superconductors with high quality factors, high operation temperatures, and high-field potentials are critical for these devices. However, surface roughness, non-stoichiometry, and impurities in Nb3Sn deposited by conventional Sn-vapor diffusion prevent them from reaching their theoretical capabilities. Here we demonstrate a seed-free electrochemical synthesis that pushes the limit of chemical and physical properties in Nb3Sn. Utilization of electrochemical Sn pre-deposits reduces the roughness of converted Nb3Sn by five times compared to typical vapor-diffused Nb3Sn. Quantitative mappings using chemical and atomic probes confirm improved stoichiometry and minimized impurity concentrations in electrochemically synthesized Nb3Sn. We have successfully applied this Nb3Sn to the large-scale 1.3 GHz SRF cavity and demonstrated ultra-low BCS surface resistances at multiple operation temperatures, notably lower than vapor-diffused cavities. Our smooth, homogeneous, high-purity Nb3Sn provides the route toward high efficiency and high fields for SRF applications under helium-free cryogenic operations.

cond-mat.mtrl-sci↗

arXiv2023

Supercell formation in epitaxial rare-earth ditelluride thin films

Square net tellurides host an array of electronic ground states and commonly exhibit charge-density-wave ordering. Here we report the epitaxy of DyTe$_{2-δ}$ on atomically flat MgO (001) using molecular beam epitaxy. The films are single phase and highly oriented as evidenced by transmission electron microscopy and X-ray diffraction measurements. Epitaxial strain is evident in films and is relieved as the thickness increases up to a value of approximately 20 unit cells. Diffraction features associated with a supercell in the films are resolved which is coupled with Te-deficiency. First principles calculations attribute the formation of this defect lattice to nesting conditions in the Fermi surface, which produce a periodic occupancy of the conducting Te square-net, and opens a band gap at the chemical potential. This work establishes the groundwork for exploring the role of strain in tuning electronic and structural phases of epitaxial square-net tellurides and related compounds.

cond-mat.mtrl-sci↗

arXiv2023

Tuning the Curie temperature of a 2D magnet/topological insulator heterostructure to above room temperature by epitaxial growth

Heterostructures of two-dimensional (2D) van der Waals (vdW) magnets and topological insulators (TI) are of substantial interest as candidate materials for efficient spin-torque switching, quantum anomalous Hall effect, and chiral spin textures. However, since many of the vdW magnets have Curie temperatures below room temperature, we want to understand how materials can be modified to stabilize their magnetic ordering to higher temperatures. In this work, we utilize molecular beam epitaxy to systematically tune the Curie temperature ($T_C$) in thin film Fe$_3$GeTe$_2$/Bi$_2$Te$_3$ from bulk-like values ($\sim$220 K) to above room temperature by increasing the growth temperature from 300 $^\circ$C to 375 $^\circ$C. For samples grown at 375 $^\circ$C, cross-sectional scanning transmission electron microscopy (STEM) reveals the spontaneous formation of different Fe$_m$Ge$_n$Te$_2$ compositions (e.g. Fe$_5$Ge$_2$Te$_2$ and Fe$_7$Ge$_6$Te$_2$) as well as intercalation in the vdW gaps, which are possible origins of the enhanced Curie temperature. This observation paves the way for developing various Fe$_m$Ge$_n$Te$_2$/TI heterostructures with novel properties.

cond-mat.mtrl-sci↗

arXiv2023

Thermodynamic route of Nb3Sn nucleation: Role of oxygen

Intermetallic Nb3Sn alloys have long been believed to form through Sn diffusion into Nb. However, our observations of significant oxygen content in Nb3Sn prompted an investigation of alternative formation mechanisms. Through experiments involving different oxide interfaces (clean HF-treated, native oxidized, and anodized), we demonstrate a thermodynamic route that fundamentally challenges the conventional Sn diffusion mechanism for Nb3Sn nucleation. Our results highlight the critical involvement of a SnOx intermediate phase. This new nucleation mechanism identifies the principles for growth optimization and new synthesis of high-quality Nb3Sn superconductors.

cond-mat.mtrl-sci↗