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David A. Muller

Publications and source records attributed to David A. Muller.

At least 91 records · Page 5Linked to original sources

Ferroelectricity in Polar ScAlN/GaN Epitaxial Semiconductor Heterostructures

Room temperature ferroelectricity is observed in lattice-matched ~18% ScAlN/GaN heterostructures grown by molecular beam epitaxy on single-crystal GaN substrates. The epitaxial films have smooth surface morphologies and high crystallinity. Pulsed current-voltage measurements confirm stable and repeatable polarization switching in such ferroelectric/semiconductor structures at several measurement conditions, and in multiple samples. The measured coercive field values are Ec~0.7 MV/cm at room temperature, with remnant polarization Pr~10 μC/cm2 for ~100 nm thick ScAlN layers. These values are substantially lower than comparable ScAlN control layers deposited by sputtering. Importantly, the coercive field of MBE ScAlN is smaller than the critical breakdown field of GaN, offering the potential for low voltage ferroelectric switching. The low coercive field ferroelectricity of ScAlN on GaN heralds the possibility of new forms of electronic and photonic devices with epitaxially integrated ferroelectric/semiconductor heterostructures that take advantage of the GaN electronic and photonic semiconductor platform, where the underlying semiconductors themselves exhibit spontaneous and piezoelectric polarization.

cond-mat.mtrl-sci↗

Emergence of a noncollinear magnetic state in twisted bilayer CrI3

The emergence of two-dimensional (2D) magnetic crystals and moiré engineering has opened the door for devising new magnetic ground states via competing interactions in moiré superlattices. Although a suite of interesting phenomena, including multi-flavor magnetic states, noncollinear magnetic states, moiré magnon bands and magnon networks, has been predicted, nontrivial magnetic ground states in twisted bilayer magnetic crystals have yet to be realized. Here, by utilizing the stacking-dependent interlayer exchange interactions in CrI3, we demonstrate in small-twist-angle bilayer CrI3 a noncollinear magnetic ground state. It consists of both antiferromagnetic (AF) and ferromagnetic (FM) domains and is a result of the competing interlayer AF coupling in the monoclinic stacking regions of the moiré superlattice and the energy cost for forming AF-FM domain walls. Above the critical twist angle of ~ 3°, the noncollinear state transitions abruptly to a collinear FM ground state. We further show that the noncollinear magnetic state can be controlled by gating through the doping-dependent interlayer AF interaction. Our results demonstrate the possibility of engineering moiré magnetism in twisted bilayer magnetic crystals, as well as gate-voltage-controllable high-density magnetic memory storage.

cond-mat.mtrl-sci↗

Lossless monochromation for electron microscopy with pulsed photoemission sources and rf cavities

Resonant radiofrequency cavities enable exquisite time-energy control of electron beams when synchronized with laser driven photoemission. We present a lossless monochromator design that exploits this fine control in the one-electron-per-pulse regime. The theoretically achievable maximum beam current on target is orders of magnitude greater than state-of-the-art monochromators for the same spatial and energy resolution. This improvement is the result of monochromating in the time domain, unconstrained by the transverse brightness of the electron source. We show analytically and confirm numerically that cavity parameters chosen to minimize energy spread perform the additional function of undoing the appreciable effect of chromatic aberration in the upstream optics. We argue that our design has significant applications in both ultra-fast and non-time-resolved microscopy, provided photoelectron sources of sufficiently small size and laser sources of sufficiently high repetition rate. Our design achieves in simulations more than two orders of magnitude reduction in beam energy spread, down to single digit meV. Overcoming the minimum probe-size limit that chromatic aberration imposes, our design clears a path for high-current, high-resolution electron beam applications at primary energies from single to hundreds of keV.

physics.acc-ph↗

Electron ptychography achieves atomic-resolution limits set by lattice vibrations

Transmission electron microscopes use electrons with wavelengths of a few picometers, potentially capable of imaging individual atoms in solids at a resolution ultimately set by the intrinsic size of an atom. Unfortunately, due to imperfections in the imaging lenses and multiple scattering of electrons in the sample, the image resolution reached is 3 to 10 times worse. Here, by inversely solving the multiple scattering problem and overcoming the aberrations of the electron probe using electron ptychography to recover a linear phase response in thick samples, we demonstrate an instrumental blurring of under 20 picometers. The widths of atomic columns in the measured electrostatic potential are now no longer limited by the imaging system, but instead by the thermal fluctuations of the atoms. We also demonstrate that electron ptychography can potentially reach a sub-nanometer depth resolution and locate embedded atomic dopants in all three dimensions with only a single projection measurement.

cond-mat.mtrl-sci↗

The Breakdown of Mott Physics at VO$_2$ Surfaces

Transition metal oxides such as vanadium dioxide (VO$_2$), niobium dioxide (NbO$_2$), and titanium sesquioxide (Ti$_2$O$_3$) are known to undergo a temperature-dependent metal-insulator transition (MIT) in conjunction with a structural transition within their bulk. However, it is not typically discussed how breaking crystal symmetry via surface termination affects the complicated MIT physics. Using synchrotron-based x-ray spectroscopy, low energy electron diffraction (LEED), low energy electron microscopy (LEEM), transmission electron microscopy (TEM), and several other experimental techniques, we show that suppression of the bulk structural transition is a common feature at VO$_2$ surfaces. Our density functional theory (DFT) calculations further suggest that this is due to inherent reconstructions necessary to stabilize the surface, which deviate the electronic structure away from the bulk d$^1$ configuration. Our findings have broader ramifications not only for the characterization of other "Mott-like" MITs, but also for any potential device applications of such materials.

cond-mat.str-el↗

Revealing the Nanostructure of Mesoporous Fuel Cell Catalyst Supports for Durable, High-Power Performance

Achieving high power performance and durability with low Pt loadings are critical challenges for proton exchange membrane fuel cells. PtCo catalysts developed on new carbon black supports show promise by simultaneously providing good oxygen reduction kinetics and local oxygen transport. We investigate the role of nanoscale morphology in the performance of these catalysts supported on accessible (HSC-e and HSC-f) and conventional (Ketjen Black) porous carbons using 3D electron tomography, nitrogen sorption, and electrochemical performance measurements. We find that the accessible porous carbons have hollow interiors with mesopores that are larger and more numerous than conventional porous carbons. However, mesopore-sized openings (>2nm width) are too rare to account for significant oxygen transport. Instead we propose the primary oxygen transport pathway into the interior is through 1-2nm microporous channels permeating the carbon. The increased mesoporosity in the accessible porous carbons results in a shorter diffusion pathlength through constrictive, tortuous micropores in the support shell leading to lower local oxygen transport resistance. In durability testing, the accessible porous carbons show faster rates of electrochemical surface area loss, likely from fewer constrictive pores that would mitigate coarsening, but maintain superior high current density performance at end of life from the improved local oxygen transport.

cond-mat.mtrl-sci↗

$γ$-phase Inclusions as Common Defects in Alloyed $β$-(Al$_x$Ga$_{1\text{-}x}$)$_2$O$_3$ and Doped $β$-Ga$_2$O$_3$ Films

$β$-Ga$_2$O$_3$ is a promising ultra-wide bandgap semiconductor whose properties can be further enhanced by alloying with Al. Here, using atomic-resolution scanning transmission electron microscopy (STEM), we find the thermodynamically-unstable $γ$-phase is a ubiquitous defect in both $β$-(Al$_x$Ga$_{1\text{-}x}$)$_2$O$_3$ films and doped $β$-Ga$_2$O$_3$ films grown by molecular beam epitaxy. For undoped $β$-(Al$_x$Ga$_{1\text{-}x}$)$_2$O$_3$ films we observe $γ$-phase inclusions between nucleating islands of the $β$-phase at lower growth temperatures (~400-600 $^{\circ}$C). In doped $β$-Ga$_2$O$_3$, a thin layer of the $γ$-phase is observed on the surfaces of films grown with a wide range of n-type dopants and dopant concentrations. The thickness of the $γ$-phase layer was most strongly correlated with the growth temperature, peaking at about 600 $^{\circ}$C. Ga interstitials are observed in $β$-phase, especially near the interface with the $γ$-phase. By imaging the same region of the surface of a Sn-doped $β$-(Al$_x$Ga$_{1\text{-}x}$)$_2$O$_3$ after ex-situ heating up to 400 $^{\circ}$C, a $γ$-phase region is observed to grow above the initial surface, accompanied by a decrease in Ga interstitials in the $β$-phase. This suggests that the diffusion of Ga interstitials towards the surface is likely the mechanism for growth of the surface $γ$-phase, and more generally that the more-open $γ$-phase may offer diffusion pathways to be a kinetically-favored and early-forming phase in the growth of Ga$_2$O$_3$.

cond-mat.mtrl-sci↗

Adsorption-Controlled Growth of Ga2O3 by Suboxide Molecular-Beam Epitaxy

This paper introduces a growth method---suboxide molecular-beam epitaxy (S-MBE)---which enables the growth of Ga2O3 and related materials at growth rates exceeding 1 micrometer per hours with excellent crystallinity in an adsorptioncontrolled regime. Using a Ga + Ga2O3 mixture with an oxygen mole fraction of x(O) = 0.4 as an MBE source, we overcome kinetic limits that had previously hampered the adsorption-controlled growth of Ga2O3 by MBE. We present growth rates up to 1.6 micrometer per hour for Ga2O3--Al2O3 heterostructures with unprecedented crystalline quality and also at unparalleled low growth temperature for this level of perfection. We combine thermodynamic knowledge of how to create molecular-beams of targeted suboxides with a kinetic model developed for the S-MBE of III-VI compounds to identify appropriate growth conditions. Using S-MBE we demonstrate the growth of phase-pure, smooth, and high-purity homoepitaxial Ga2O3 films that are thicker than 4 micrometer. With the high growth rate of S-MBE we anticipate a significant improvement to vertical Ga2O3-based devices. We describe and demonstrate how this growth method can be applied to a wide-range of oxides. S-MBE rivals leading synthesis methods currently used for the production of Ga2O3-based devices.

cond-mat.mtrl-sci↗

The Exit-Wave Power-Cepstrum Transform for Scanning Nanobeam Electron Diffraction: Robust Strain Mapping at Subnanometer Resolution and Subpicometer Precision

Scanning nanobeam electron diffraction (NBED) with fast pixelated detectors is a valuable technique for rapid, spatially resolved mapping of lattice structure over a wide range of length scales. However, intensity variations caused by dynamical diffraction and sample mistilts can hinder the measurement of diffracted disk centers as necessary for quantification. Robust data processing techniques are needed to provide accurate and precise measurements for complex samples and non-ideal conditions. Here we present an approach to address these challenges using a transform, called the exit wave power cepstrum (EWPC), inspired by cepstral analysis in audio signal processing. The EWPC transforms NBED patterns into real-space patterns with sharp peaks corresponding to inter-atomic spacings. We describe a simple analytical model for interpretation of these patterns that cleanly decouples lattice information from the intensity variations in NBED patterns caused by tilt and thickness. By tracking the inter-atomic spacing peaks in EWPC patterns, strain mapping is demonstrated for two practical applications: mapping of ferroelectric domains in epitaxially strained PbTiO3 films and mapping of strain profiles in arbitrarily oriented core-shell Pt-Co nanoparticle fuel-cell catalysts. The EWPC transform enables lattice structure measurement at sub-pm precision and sub-nm resolution that is robust to small sample mistilts and random orientations.

cond-mat.mtrl-sci↗

Tuning the convergence angle for optimum STEM performance

The achievable instrumental performance of a scanning transmission electron microscope (STEM) is determined by the size and shape of the incident electron probe. The most important optical factor in achieving the optimum probe profile is the radius of the probe-forming aperture, which determines the convergence semi-angle of the illumination. What is often overlooked however is that small deviations from this optimum can degrade both the resolution and interpretability of image contrast. A 30% error in aperture radius can lead to a factor of 2 contrast reduction in typical lattice spacings, and a 5 Å error in the thickness measurement of thin layers (such as gate oxides). Theoretical calculations of the optimum convergence angles, from a wave-optical consideration of the probe forming conditions, are explained and their consequences discussed. An experimental approach to the measurement and tuning of the convergence angle is then introduced. This is intended for uncorrected electron microscopes. For corrected instruments, Cs=0, and Cc usually determines the choice of aperture - see e.g. ULTRAMICROSCOPY 108, (2008) 1454-1466

cond-mat.mtrl-sci↗

Observation of strong bulk damping-like spin-orbit torque in chemically disordered ferromagnetic single layers

Strong damping-like spin-orbit torque (τDL) has great potential for enabling ultrafast energy-efficient magnetic memories, oscillators, and logic. So far, the reported τDL exerted on a thin-film magnet must result from an externally generated spin current or from an internal non-equilibrium spin polarization in noncentrosymmetric GaMnAs single crystals. Here, we for the first time demonstrate a very strong, unexpected τDL from current flow within ferromagnetic single layers of chemically disordered, face-centered-cubic CoPt. We establish that the novel τDL is a bulk effect, with the strength per unit current density increasing monotonically with the CoPt thickness, and is insensitive to the presence or absence of spin sinks at the CoPt surfaces. This τDL most likely arises from a net transverse spin polarization associated with a strong spin Hall effect (SHE), while there is no detectable long-range asymmetry in the material. These results broaden the scope of spin-orbitronics and provide a novel avenue for developing single-layer-based spin-torque memory, oscillator, and logic technologies.

cond-mat.mtrl-sci↗

Crystal orientation dictated epitaxy of ultrawide bandgap 5.4-8.6 eV $α$-(AlGa)$_2$O$_3$ on m-plane sapphire

Ultra-wide bandgap semiconductors are ushering in the next generation of high power electronics. The correct crystal orientation can make or break successful epitaxy of such semiconductors. Here it is discovered that single-crystalline layers of $α$-(AlGa)$_2$O$_3$ alloys spanning bandgaps of 5.4 - 8.6 eV can be grown by molecular beam epitaxy. The key step is found to be the use of m-plane sapphire crystal. The phase transition of the epitaxial layers from the $α$- to the narrower bandgap $β$-phase is catalyzed by the c-plane of the crystal. Because the c-plane is orthogonal to the growth front of the m-plane surface of the crystal, the narrower bandgap pathways are eliminated, revealing a route to much wider bandgap materials with structural purity. The resulting energy bandgaps of the epitaxial layers span a range beyond the reach of all other semiconductor families, heralding the successful epitaxial stabilization of the largest bandgap materials family to date.

physics.app-ph↗

Dimensionality-induced change in topological order in multiferroic oxide superlattices

We construct ferroelectric (LuFeO3)m/(LuFe2O4) superlattices with varying index m to study the effect of confinement on topological defects. We observe a thickness-dependent transition from neutral to charged domain walls and the emergence of fractional vortices. In thin LuFeO3 layers, the volume fraction of domain walls grows, lowering the symmetry from P63cm to P3c1 before reaching the non-polar P63/mmc state, analogous to the high-temperature ferroelectric to paraelectric transition. Our study shows how dimensional confinement stabilizes textures beyond those in bulk ferroelectric systems.

cond-mat.mtrl-sci↗

Overcoming information reduced data and experimentally uncertain parameters in ptychography with regularized optimization

The overdetermination of the mathematical problem underlying ptychography is reduced by a host of experimentally more desirable settings. Furthermore, reconstruction of the sample-induced phase shift is typically limited by uncertainty in the experimental parameters and finite sample thicknesses. Presented is a conjugate gradient descent algorithm, regularized optimization for ptychography (ROP), that recovers the partially known experimental parameters along with the phase shift, improves resolution by incorporating the multislice formalism to treat finite sample thicknesses, and includes regularization in the optimization process, thus achieving reliable results from noisy data with severely reduced and underdetermined information.

eess.SP↗

Operando Control of Skyrmion Density in a Lorentz Transmission Electron Microscope with Current Pulses

Magnetic skyrmions hold promise for spintronic devices. To explore the dynamical properties of skyrmions in devices, a nanoscale method to image spin textures in response to a stimulus is essential. Here, we apply a technique for operando electrical current pulsing of chiral magnetic devices in a Lorentz transmission electron microscope. In ferromagnetic multilayers with interfacial Dzyaloshinskii-Moriya interaction (DMI), we study the creation and annihilation of skyrmions localized by point-like pinning sites due to defects. Using a combination of experimental and micromagnetic techniques, we establish a thermal contribution for the creation and annihilation of skyrmions in our study. Our work reveals a mechanism for controlling skyrmion density, which enables an examination of skyrmion magnetic field stability as a function of density. We find that high-density skyrmion states are more stable than low-density states or isolated skyrmions resisting annihilation over a magnetic field range that increases monotonically with density.

cond-mat.mes-hall↗

Bidirectional Self-Folding with Atomic Layer Deposition Nanofilms for Microscale Origami

Origami design principles are scale invariant and enable direct miniaturization of origami structures provided the sheets used for folding have equal thickness to length ratios. Recently, seminal steps have been taken to fabricate microscale origami using unidirectionally actuated sheets with nanoscale thickness. Here, we extend the full power of origami-inspired fabrication to nanoscale sheets by engineering bidirectional folding with 4 nm thick atomic layer deposition (ALD) SiNx-SiO2 bilayer films. Strain differentials within these bilayers result in bending, producing microscopic radii of curvature. We lithographically pattern these bilayers and localize the bending using rigid panels to fabricate a variety of complex micro-origami devices. Upon release, these devices self-fold according to prescribed patterns. Our approach combines planar semiconductor microfabrication methods with computerized origami design, making it easy to fabricate and deploy such microstructures en masse. These devices represent an important step forward in the fabrication and assembly of deployable micromechanical systems that can interact with and manipulate micro- and nanoscale environments.

physics.app-ph↗

Electron tomography for functional nanomaterials

Modern nanomaterials contain complexity that spans all three dimensions - from multigate semiconductors to clean energy nanocatalysts to complex block copolymers. For nanoscale characterization, it has been a long-standing goal to observe and quantify the three-dimensional (3D) structure - not just surfaces, but the entire internal volume and the chemical arrangement. Electron tomography estimates the complete 3D structure of nanomaterials from a series of two-dimensional projections taken across many viewing angles. Since its first introduction in 1968, electron tomography has progressed substantially in resolution, dose, and chemical sensitivity. In particular, scanning transmission electron microscope tomography has greatly enhanced the study of 3D nanomaterials by providing quantifiable internal morphology and spectroscopic detection of elements. Combined with recent innovations in computational reconstruction algorithms and 3D visualization tools, scientists can interactively dissect volumetric representations and extract meaningful statistics of specimens. This article highlights the maturing field of electron tomography and the widening scientific applications that utilize 3D structural, chemical, and functional imaging at the nanometer and subnanometer length scales.

physics.app-ph↗

Imaging Polarity in Two Dimensional Materials by Breaking Friedel's Law

Friedel's law guarantees an inversion-symmetric diffraction pattern for thin, light materials where a kinematic approximation or a single-scattering model holds. Typically, breaking Friedel symmetry is ascribed to multiple scattering events within thick, non-centrosymmetric crystals. However, two-dimensional (2D) materials such as a single monolayer of MoS$_2$ can also violate Friedel's law, with unexpected contrast between conjugate Bragg peaks. We show analytically that retaining higher order terms in the power series expansion of the scattered wavefunction can describe the anomalous contrast between $hkl$ and $\overline{hkl}$ peaks that occurs in 2D crystals with broken in-plane inversion symmetry. These higher-order terms describe multiple scattering paths starting from the same atom in an atomically thin material. Furthermore, 2D materials containing heavy elements, such as WS$_2$, always act as strong phase objects, violating Friedel's law no matter how high the energy of the incident electron beam. Experimentally, this understanding can enhance diffraction-based techniques to provide rapid imaging of polarity, twin domains, in-plane rotations, or other polar textures in 2D materials.

cond-mat.mtrl-sci↗