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We present data for epitaxial thin films of the prototypical entropy-stabilized oxide (ESO), Mg0.2Ni0.2Co0.2Cu0.2Zn0.2O, that reveals a systematic trend in lattice parameter and properties as a function of substrate temperature during film growth with negligible changes in microstructure. A larger net Co valence in films grown at substrate temperatures below 350 °C results in a smaller lattice parameter, a smaller optical band gap, and stronger magnetic exchange bias. Observation of this phenomena suggests a complex interplay between thermodynamics and kinetics during ESO synthesis; specifically thermal history, oxygen chemical potential, and entropy. In addition to the compositional degrees of freedom available to ESO systems, subtle nuances in atomic structure at constant metallic element proportions can strongly influence properties, simultaneously complicating physical characterization and providing opportunities for property tuning and development.

A memristor array has emerged as a potential computing hardware for artificial intelligence (AI). It has an inherent memory effect that allows information storage in the form of easily programmable electrical conductance, making it suitable for efficient data processing without shuttling of data between the processor and memory. To realize its full potential for AI applications, fine-tuning of internal device dynamics is required to implement a network system that employs dynamic functions. Here, we provide a perspective on multicationic entropy-stabilized oxides as a widely tunable materials system for memristor applications. We highlight the potential for efficient data processing in machine learning tasks enabled by the implementation of "task specific" neural networks that derive from this material tunability. [ABSTRACT FROM AUTHOR]

The development of high performance wide-bandgap AlGaN channel transistors with high current densities and reduced Ohmic losses necessitates extremely highly doped, high Al content AlGaN epilayers for regrown source/drain contact regions. In this work, we demonstrate the achievement of semi-metallic conductivity in silicon (Si) doped N-polar Al0.6Ga0.4N grown on C-face 4H-SiC substrates by molecular beam epitaxy. Under optimized conditions, the AlGaN epilayer shows smooth surface morphology and a narrow photoluminescence spectral linewidth, without the presence of any secondary peaks. A favorable growth window is identified wherein the free electron concentration reaches as high as ∼1.8 × 1020 cm−3 as obtained from Hall measurements, with a high mobility of 34 cm2/V·s, leading to a room temperature resistivity of only 1 mΩ·cm. Temperature-dependent Hall measurements show that the electron concentration, mobility, and sheet resistance do not depend on temperature, clearly indicating dopant Mott transition to a semi-metallic state, wherein the activation energy (Ea) falls to 0 meV at this high value of Si doping for the AlGaN films. This achievement of semi-metallic conductivity in Si doped N-polar high Al content AlGaN is instrumental for advancing ultrawide bandgap electronic and optoelectronic devices. [ABSTRACT FROM AUTHOR]

The Nernst effect describes a linear relationship between orthogonal components of a magnetic field, a temperature gradient, and a resulting transverse electric field. A non-local electrical measurement, where injection and detection are physically separated on the specimen, serves as a versatile and effective platform for measuring spin and thermal effects due to the avoided interference with a charge current directly. Here, we quantify the Nernst coefficient of Pt, a common material for spin injection in non-local geometries, by a non-local electrical measurement under modulated temperature and magnetic field and finite element analysis for modeling heat transfer. We determine the Nernst coefficient of Pt from room temperature (8.56 nV K − 1 T − 1 ) to 10 K (29.3 nV K − 1 T − 1 ). Beyond the quantification of the Nernst coefficient, our results show that careful consideration of the thermal properties of the thermal sink and electrode materials is needed when making an interpretation of non-local electrical measurements. [ABSTRACT FROM AUTHOR]

Entropy-stabilized oxides are single-phase, multicomponent oxides that are stabilized by a large entropy of mixing, ΔS, overcoming a positive enthalpy. Due to the −TΔS term in the Gibbs' free energy, G, it can be hypothesized that entropy-stabilized oxides demonstrate a robust thermal stability. Here, we investigate the high temperature stability (1300–1700 °C) of the prototypical entropy-stabilized rocksalt oxide (MgCoNiCuZn)0.2O in air. We find that at temperatures >1300 °C, the material gradually loses Cu and Zn with increasing temperature. Cu is lost through a selective melting as a Cu-rich liquid phase is formed. Zn is sublimed from the rocksalt phase at approximately similar temperatures to those corresponding to the Cu loss, significantly below both the melting temperature of ZnO and its solubility limit in a rocksalt phase. The elemental loss progressively reduces the entropy of mixing and results in a multiphase solid upon quenching to room temperature. We posit that the high-temperature solubility of Cu and Zn is correlated providing further evidence for entropic stabilization over general solubility arguments. [ABSTRACT FROM AUTHOR]

Functional thin film superlattices with stability in extreme environments can lead to transformative performance in optical and thermal applications such as thermophotovoltaics. In this work, key issues associated with defects that prevent layer-by-layer growth in epitaxial, low-miscibility oxide superlattices are investigated. Layer protrusions, approximately 8 nm wide and 3 nm thick, arise from a strain relaxation mechanism in 8 nm bilayer superlattices of Ba(Zr0.5Hf0.5)O3/MgO and propagate through the subsequent superlattice layers forming an inverted pyramid structure that is spatially phase offset from the matrix. The density and size of these defects scales with the number of interfaces in the sample, indicating that surface roughness during growth is a significant factor in the formation of these defects. In situ high temperature transmission electron microscopy (1000 °C, in vacuo) measurement reveals that phase decomposition of Ba(Zr0.5Hf0.5)O3 and decoherence of the superlattice is nucleated by these defects. This work highlights that achieving optimum growth conditions is imperative to the synthesis of single-crystalline superlattices with sharp interfaces for optimized performance in extreme environments. [ABSTRACT FROM AUTHOR]

Ferrimagnetic insulators with perpendicular magnetic anisotropy are of particular interest for spintronics due to their ability to mitigate current shunting in spin–orbit torque heterostructures and enable low switching energy, high-density storage magnetic devices. Rare earth iron garnet Tm3Fe5O12 (TmIG) is one such material where prior studies have shown that the negative magnetostriction coefficient and isotropic in-plane tensile strain enable the magnetoelastic anisotropy to overcome the demagnetization energy and stabilize perpendicular magnetic anisotropy. However, the investigation of the tunability of the magnetoelastic anisotropy between thin films that possess perpendicular magnetization and quantification of the magnetoelastic constants has not been reported. Here, we quantify the evolution of magnetic anisotropy in (111)-oriented, epitaxial, 17 nm thick thin films of TmIG using a systematic variation of in-plane epitaxial strain (ranging 0.49%–1.83%) imposed by a suite of commercially available garnet substrates. Within the confines of the imposed strain range and deposition condition, the distortion from cubic symmetry is found to be approximately linear within the in-plane strain. The magnetic anisotropy field can be tuned by a factor of 14 in this strain range. The magnetoelastic anisotropy constant, B2, is found to be approximately constant (∼2500 kJ m−3) and more than 2× larger than the reported bulk value (∼1200 kJ m−3) for a cubic distortion between 90.17° and 90.71°. B2 is found to decrease at cubic distortions of 90.74° and larger. Our results highlight strain engineering, and its limitations, for control of perpendicular magnetic anisotropy. [ABSTRACT FROM AUTHOR]

Magnetoactive soft materials, typically composed of magnetic particles dispersed in a soft polymer matrix, are finding many applications in soft robotics due to their reversible and remote shape transformations under magnetic fields. To achieve complex shape transformations, anisotropic, and heterogeneous magnetization profiles must be programmed in the material. However, once programmed and assembled, magnetic soft actuators cannot be easily reconfigured, repurposed, or repaired, which limits their application, their durability, and versatility in their design. Here, magnetoactive soft composites are developed from squid‐derived biopolymers and NdFeB microparticles with tunable ferromagnetic and thermomechanical properties. By leveraging reversible crosslinking nanostructures in the biopolymer matrix, a healing‐assisted assembly process is developed that allows for on‐demand reconfiguration and magnetic reprogramming of magnetoactive composites. This concept in multi‐material modular actuators is demonstrated with programmable deformation modes, self‐healing properties to recover their function after mechanical damage, and shape‐memory behavior to lock in their preferred configuration and un‐actuated catch states. These dynamic magnetic soft composites can enable the modular design and assembly of new types of magnetic actuators, not only eliminating device vulnerabilities through healing and repair but also by providing adaptive mechanisms to reconfigure their function on demand. [ABSTRACT FROM AUTHOR]

Author(s): Julia A. Mundy [1]; Charles M. Brooks [2]; Megan E. Holtz [1]; Jarrett A. Moyer [3]; Hena Das [1]; Alejandro F. Rbola [1]; John T. Heron [2, 4]; James [...]

Since the resurgence of multiferroics research, significant advancement has been made in the theoretical and experimental investigation of the electric field control of magnetization, magnetic anisotropy, magnetic phase, magnetic domains, and Curie temperature in multiferroic heterostructures. As a result of these advances, multiferroic heterostructures are on a trajectory to impact spintronics applications through the significantly reduced energy consumption per unit area for magnetization switching (1–500 μJ cm−2) when compared to that of current-driven magnetization switching (0.2–10 mJ cm−2). Considering this potential impact, it becomes necessary to understand magnetoelectric switching dynamics and characteristic switching times. The body of experimental work investigating magnetoelectric switching dynamics is rather limited, with the majority of room temperature converse magnetoelectric switching measurements reported having employed relatively long voltage pulses. Recently, however, the field has started to consider the kinetics of the switching path in multiferroic (and ferroelectric) switching. Excitingly, the results are challenging our understanding of switching processes while offering new opportunities to engineer the magnetoelectric effect. Considering the prospects of multiferroics for beyond-CMOS applications and the possible influence on operational speed, much remains to be understood regarding magnetoelectric switching kinetics and dynamics, particularly at reduced dimensions and under the influence of boundary effects resulting from strain, electrostatics, and orientation. In this article, we review magnetoelectric switching in multiferroic heterostructures for the electric field control of magnetism. We then offer perspectives moving toward the goal of low energy-delay spintronics for computational applications. [ABSTRACT FROM AUTHOR]

Rutile compounds have exotic functional properties that can be applied for various electronic applications; however, the limited availability of epitaxial substrates has restricted the study of rutile thin films to a limited range of lattice parameters. Here, rutile GeO2 is demonstrated as a new rutile substrate with lattice parameters of a = 4.398 Å and c = 2.863 Å. Rutile GeO2 single crystals up to 4 mm in size are grown by the flux method. X-ray diffraction reveals high crystallinity with a rocking curve having a full width half-maximum of 0.0572°. After mechanical polishing, a surface roughness of less than 0.1 nm was obtained, and reflection high-energy electron diffraction shows a crystalline surface. Finally, epitaxial growth of (110)-oriented TiO2 thin films on GeO2 substrates was demonstrated using molecular beam epitaxy. Templated by rutile GeO2 substrates, our findings open the possibility of stabilizing new rutile thin films and strain states for the tuning of physical properties. [ABSTRACT FROM AUTHOR]

Ultrawide-band-gap (UWBG) semiconductors are promising for fast, compact, and energy-efficient power-electronics devices. Their wider band gaps result in higher breakdown electric fields that enable high-power switching with a lower energy loss. Yet, the leading UWBG semiconductors suffer from intrinsic materials' limitations with regard to their doping asymmetry that impedes their adoption in CMOS technology. Improvements in the ambipolar doping of UWBG materials will enable a wider range of applications in power electronics as well as deep-UV optoelectronics. These advances can be accomplished through theoretical insights on the limitations of current UWBG materials coupled with the computational prediction and experimental demonstration of alternative UWBG semiconductor materials with improved doping and transport properties. As an example, we discuss the case of rutile GeO2 (r-GeO2), a water-insoluble GeO2 polytype, which is theoretically predicted to combine an ultra-wide gap with ambipolar dopability, high carrier mobilities, and a higher thermal conductivity than β-Ga2O3. The subsequent realization of single-crystalline r-GeO2 thin films by molecular beam epitaxy provides the opportunity to realize r-GeO2 for electronic applications. Future efforts toward the predictive discovery and design of new UWBG semiconductors include advances in first-principles theory and high-performance computing software, as well as the demonstration of controlled doping in high-quality thin films with lower dislocation densities and optimized film properties. [ABSTRACT FROM AUTHOR]

We report on the demonstration of ferroelectricity in ScxAl1-xN grown by molecular beam epitaxy on GaN templates. Distinct polarization switching is unambiguously observed for ScxAl1-xN films with Sc contents in the range of 0.14–0.36. Sc0.20Al0.80N, which is nearly lattice-matched with GaN, exhibiting a coercive field of ∼ 4.2 MV/cm at 10 kHz and a remnant polarization of ∼135 μC/cm2. After electrical poling, Sc0.20Al0.80N presents a polarization retention time beyond 105 s. No obvious fatigue behavior can be found with up to 3 × 105 switching cycles. The work reported here is more than a technical achievement. The realization of ferroelectric single-crystalline III–V semiconductors by molecular beam epitaxy promises a thickness scaling into the nanometer regime and makes it possible to integrate high-performance ferroelectric functionality with well-established semiconductor platforms for a broad range of electronic, optoelectronic, and photonic device applications. [ABSTRACT FROM AUTHOR]

Memristors have emerged as transformative devices to enable neuromorphic and in‐memory computing, where success requires the identification and development of materials that can overcome challenges in retention and device variability. Here, high‐entropy oxide composed of Zr, Hf, Nb, Ta, Mo, and W oxides is first demonstrated as a switching material for valence change memory. This multielement oxide material provides uniform distribution and higher concentration of oxygen vacancies, limiting the stochastic behavior in resistive switching. (Zr, Hf, Nb, Ta, Mo, W) high‐entropy‐oxide‐based memristors manifest the "cocktail effect," exhibiting comparable retention with HfO2‐ or Ta2O5‐based memristors while also demonstrating the gradual conductance modulation observed in WO3‐based memristors. The electrical characterization of these high‐entropy‐oxide‐based memristors demonstrates forming‐free operation, low device and cycle variability, gradual conductance modulation, 6‐bit operation, and long retention which are promising for neuromorphic applications. [ABSTRACT FROM AUTHOR]

We propose a heterostructure device comprised of magnets and piezoelectrics, which significantly improves the delay and the energy dissipation of an all-spin logic (ASL) device. This paper studies and models the physics of the device, illustrates its operation, and benchmarks its performance using SPICE simulations. We show that the proposed device maintains low-voltage operation, nonreciprocity, nonvolatility, cascadability, and thermal reliability of the original ASL device. Moreover, by utilizing the deterministic switching of a magnet from the saddle point of the energy profile, the device is more efficient in terms of energy and delay and is robust to thermal fluctuations. The results of simulations show that compared to ASL devices, the proposed device achieves $21\times $ shorter delay and $27\times $ lower energy dissipation per bit for a 32-bit arithmetic-logic unit. [ABSTRACT FROM AUTHOR]

Recent experiments have shown the ability to introduce an anisotropy energy to the energy landscape of a thin-film nanomagnet through the use of mechanical strain. Assuming this strain-induced anisotropy is large enough, the low-energy state of the nanomagnet is altered and can be used to initialize the magnetization along a given axis. Utilizing this effect, we propose a more energy efficient method of nanomagnet reversal through spin-transfer torque (STT). This is accomplished by first initializing the magnetization to a high-energy state and then applying a short current pulse to nudge the magnetization in the appropriate energy basin. Using extensive numerical simulations, we qualitatively analyze this type of reversal and find the optimal parameters for reliable functionality while in the presence of thermal noise. We demonstrate that despite negating the initial portion of nominal STT reversal, where the STT must fight against the damping torque of the initial energy-basin, the magnitude of spin current required for our proposed strain-mediated reversal is equivalent to the nominal case. However, the strain-meditated reversal is beneficial by minimizing the spin-current pulsewidth necessary for reliable operation allowing for large energy savings. Assuming the strain-anisotropy is significantly larger than the nanomagnet’s internal free-axis anisotropy, strain-mediated reversals offer a 10 \times energy reduction over nominal STT reversals. [ABSTRACT FROM AUTHOR]

The effect of partial substitution of titanium for cobalt on 3b sites in Li1+z(NixMnxCo1-2x-yTiy)O2 (x = 1/3, 0.4) cathode materials (NMCs) has been investigated for this study. Materials were prepared by glycine-nitrate combustion and co-precipitation methods and solid solutions were observed over a narrow substitution range limited to below about y = 0.07 for both the x = 1/3 and x = 0.4 series, although this depended on the synthesis technique. Increased discharge capacities, lower first cycle inefficiencies and better cycling behavior were observed for several of the Ti-substituted compositions in electrochemical cells. The improved first cycle efficiencies allow higher discharge capacities to be obtained between normal voltage limits, which partly explain the observations. Results from synchrotron X-ray diffraction also indicate that Ti substitution leads to a decreased cell volume change during deintercalation of lithium, which contributes to the improved cycling performance. Magnetic measurements suggest that reduction of some Mn4+ to Mn3+ compensates for the aliovalent substitution in as-made lithium-stoichiometric materials. [ABSTRACT FROM AUTHOR]

We report an initial experimental survey of spin Hall torques generated by the rare-earth metals Gd, Dy, Ho, and Lu, along with comparisons to first-principles calculations of their spin Hall conductivities. Using spin torque ferromagnetic resonance (ST-FMR) measurements and dc-biased ST-FMR, we estimate lower bounds for the spin Hall torque ratio, ξSH, of ≈0.04 for Gd, ≈0.05 for Dy, ≈0.14 for Ho, and ≈0.014 for Lu. The variations among these elements are qualitatively consistent with results from first principles [density-functional theory (DFT) in the local density approximation with a Hubbard-U correction]. The DFT calculations indicate that the spin Hall conductivity is enhanced by the presence of the partially filled ƒ orbitals in Dy and Ho, which suggests a strategy to further strengthen the contribution of the ƒ orbitals to the spin Hall effect by shifting the electron chemical potential. [ABSTRACT FROM AUTHOR]

The carrier effective mass plays a crucial role in modern electronic, optical, and catalytic devices and is fundamentally related to key properties of solids such as the mobility and density of states. Here we demonstrate a method to deterministically engineer the effective mass using spatial confinement in metallic quantum wells of the transition metal oxide IrO2. Using a combination of in situ angle-resolved photoemission spectroscopy measurements in conjunction with precise synthesis by oxide molecular-beam epitaxy, we show that the low-energy electronic subbands in ultrathin films of rutile IrO2 have their effective masses enhanced by up to a factor of 6 with respect to the bulk. The origin of this strikingly large mass enhancement is the confinement-induced quantization of the highly nonparabolic, three-dimensional electronic structure of IrO2 in the ultrathin limit. This mechanism lies in contrast to that observed in other transition metal oxides, in which mass enhancement tends to result from complex electron-electron interactions and is difficult to control. Our results demonstrate a general route towards the deterministic enhancement and engineering of carrier effective masses in spatially confined systems, based on an understanding of the three-dimensional bulk electronic structure. [ABSTRACT FROM AUTHOR]

Rashba spin current generation emerges in heterostructures of ferromagnets and transition metal dichalcogenides (TMDs) due to an interface polarization and associated inversion symmetry breaking. Recent work exploring the synthesis and transfer of epitaxial films on the top of low layer count 2D materials reveals that atomic potentials from the underlying substrate interface are not completely screened. The extension of this transparency effect to other interfacial phenomena, such as the Rashba effect and associated spin torques, has not yet been demonstrated. Here, we report enhanced spin transfer torques from the Rashba spin current in heterostructures of permalloy (Py) and WSe 2 . We show that insertion of up to two monolayers of WSe 2 enhances the spin transfer torques in a Rashba system by up to 3×, without changing the fieldlike Rashba spin-orbit torque (SOT), a measure of interface polarization. Our results indicate that low layer count TMD films can be used as an interfacial "scattering promoter" in heterostructure interfaces without quenching the original polarization.

The carrier effective mass plays a crucial role in modern electronic, optical, and catalytic devices and is fundamentally related to key properties of solids such as the mobility and density of states. Here we demonstrate a method to deterministically engineer the effective mass using spatial confinement in metallic quantum wells of the transition metal oxide IrO_{2}. Using a combination of in situ angle-resolved photoemission spectroscopy measurements in conjunction with precise synthesis by oxide molecular-beam epitaxy, we show that the low-energy electronic subbands in ultrathin films of rutile IrO_{2} have their effective masses enhanced by up to a factor of 6 with respect to the bulk. The origin of this strikingly large mass enhancement is the confinement-induced quantization of the highly nonparabolic, three-dimensional electronic structure of IrO_{2} in the ultrathin limit. This mechanism lies in contrast to that observed in other transition metal oxides, in which mass enhancement tends to result from complex electron-electron interactions and is difficult to control. Our results demonstrate a general route towards the deterministic enhancement and engineering of carrier effective masses in spatially confined systems, based on an understanding of the three-dimensional bulk electronic structure.

Here, we present a procedure for the synthesis of bulk and thin film multicomponent (Mg0.25(1-x)CoxNi0.25(1-x)Cu0.25(1-x)Zn0.25(1-x))O (Co variant) and (Mg0.25(1-x)Co0.25(1-x)Ni0.25(1-x)CuxZn0.25(1-x))O (Cu variant) entropy-stabilized oxides. Phase pure and chemically homogeneous (Mg0.25(1-x)CoxNi0.25(1-x)Cu0.25(1-x)Zn0.25(1-x))O (x = 0.20, 0.27, 0.33) and (Mg0.25(1-x)Co0.25(1-x)Ni0.25(1-x)CuxZn0.25(1-x))O (x = 0.11, 0.27) ceramic pellets are synthesized and used in the deposition of ultra-high quality, phase pure, single crystalline thin films of the target stoichiometry. A detailed methodology for the deposition of smooth, chemically homogeneous, entropy-stabilized oxide thin films by pulsed laser deposition on (001)-oriented MgO substrates is described. The phase and crystallinity of bulk and thin film materials are confirmed using X-ray diffraction. Composition and chemical homogeneity are confirmed by X-ray photoelectron spectroscopy and energy dispersive X-ray spectroscopy. The surface topography of thin films is measured with scanning probe microscopy. The synthesis of high quality, single crystalline, entropy-stabilized oxide thin films enables the study of interface, size, strain, and disorder effects on the properties in this new class of highly disordered oxide materials.

We describe a hybrid pixel array detector (electron microscope pixel array detector, or EMPAD) adapted for use in electron microscope applications, especially as a universal detector for scanning transmission electron microscopy. The 128×128 pixel detector consists of a 500 µm thick silicon diode array bump-bonded pixel-by-pixel to an application-specific integrated circuit. The in-pixel circuitry provides a 1,000,000:1 dynamic range within a single frame, allowing the direct electron beam to be imaged while still maintaining single electron sensitivity. A 1.1 kHz framing rate enables rapid data collection and minimizes sample drift distortions while scanning. By capturing the entire unsaturated diffraction pattern in scanning mode, one can simultaneously capture bright field, dark field, and phase contrast information, as well as being able to analyze the full scattering distribution, allowing true center of mass imaging. The scattering is recorded on an absolute scale, so that information such as local sample thickness can be directly determined. This paper describes the detector architecture, data acquisition system, and preliminary results from experiments with 80-200 keV electron beams.