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At least 307 records · Page 17

Evolution of Oxygen Ligands upon Large Redox Swings of Li 3 IrO 4

The limits of intercalation electrochemistry continue to be tested in the quest for ever increasing gains in the storage capability of Li-ion cathodes. The subsequent push for multi-electron reactivity has led to the recognition of the extremely versatile role of oxide ligands in charge compensation when there is a large redox swing. Li 3 IrO 4 is a unique model of such activity because it can reversibly cycle between Li 1 IrO 4 and Li 4.7 IrO 4 . In this study, X-ray spectroscopy, magnetic measurements and computational simulations uncover the evolution of O states in the different steps, compared to the involvement of Ir. While the process between Li 1 IrO 4 and Li 3 IrO 4 is dominated by the unconventional lattice oxygen redox, the process between Li 3 IrO 4 and Li 4.7 IrO 4 involves a conventional change of the formal oxidation state of Ir, which affects O due to the high covalency. The O states of Li 3 IrO 4 exhibit a very high reversibility after the whole 3.7-electron process, completely restoring the pristine state.

25 ENERGY STORAGE↗

Nonlinear Modeling of Macroscopic Plasma Dynamics Final Scientific Report May 1, 2006 – April 30, 2018

The project entitled, "Nonlinear Modeling of Macroscopic Plasma Dynamics," applied numerical computation to solve mathematical models of plasma behavior in laboratory systems. Plasma is the state of matter with sufficiently large internal energy density such that electrons dissociate from atoms to form gas of electrically charged particles. It occurs naturally in stars, planetary magnetospheres, and interstellar and intergalactic media. It is also used for industrial purposes and in lighting. Fusion energy science seeks to create and sustain plasma conditions where atomic nuclei fuse to create energy that can be captured for power production. Many laboratory experiments for this effort use magnetic field to contain plasma and to thermally insulate it from its surroundings. Possible plasma dynamics in magnetized systems include collective behavior over spatial scales that are comparable to the configuration size, and these dynamics often include evolution of the magnetic field that is used for confinement. Solving the mathematical models that describe these dynamics in specific experiments often requires computer simulations, as done in this project. This project analyzed plasma magnetic relaxation dynamics in the laboratory configurations known as the reversed-field pinch (RFP), the spheromak, and the spherical torus (ST). It also developed capabilities for modeling disruptive plasma dynamics in the tokamak, which has achieved the highest performance for magnetized plasma and is the design of the large international ITER experiment (https://www.iter.org) that is under construction and is expected to be the first to achieve self-heating conditions. Dynamic evolution to states of low energy, the aforementioned magnetic relaxation, is known to be important for generating the RFP and spheromak configurations. Nonlinear computational modeling with the Non-Ideal Magnetohydrodynamics with Rotation, Open Discussion code (NIMROD, https://nimrodteam.org) was applied to understand specific aspects of magnetic relaxation in RFPs, spheromaks, and STs. The RFP study considered how the nonlinear transfer of power among different fluctuation harmonics is altered due to the application of pulses of electric field, as done experimentally in the Madison Symmetric Torus RFP device at the University of Wisconsin-Madison. It also investigated the separation of electron and ion dynamics, known as two-fluid effects, including effects on the evolution of the plasma flow profile. The spheromak study considered the influence of these two-fluid effects in conditions relevant to the Sustained Spheromak Experiment (SSPX), formerly at Lawrence Livermore National Laboratory. Our study found that two-fluid effects enhance stability with respect to interchange in SSPX-relevant conditions, but having a complete model with two-fluid effects in separate electron and ion temperature equations is important. The study for STs focused on plasma startup in the Pegasus Toroidal Experiment at UW-Madison, which uses DC voltage applied through a small plasma gun. The simulations show how the resulting helical current stream relaxes through repetitive merging, forming current rings that accumulate into a tokamak-like configuration. Analytical theory was also developed to help explain behavior that was observed in the RFP and spheromak computations. Although the tokamak configuration has outperformed other magnetic confinement configurations, it has a tendency to undergo discharge-terminating dynamics that release energy onto plasma-facing surfaces and exert electromechanical forces on magnetic coils and structures. Our efforts have improved NIMROD's capabilities to model tokamak disruption by incorporating a resistive wall model that can be applied to axisymmetric, as well as asymmetric, distortions of the magnetic field configuration. Computations addressed whether mathematical conditions applied to plasma flow at the wall influence disruptive dynamics.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Controlling reversible phase transitions in rare-earth nickelates for novel memory devices

Resistive switching in correlated complex oxides is lucrative for emerging applications in neuromorphic computing, and densely scaled non-volatile memory. Electrical conductance of such complex oxides can be controllable switched across multiple orders of magnitude by either (a) electroforming a conduction channel (e.g., in tungsten oxide), or (b) inducing Mott-Hubbard transition (e.g., in rare-earth nickelates)– both via controlled migration of defects (such as oxygen vacancies) under applied bias. Nevertheless, the promise of such defect-driven electronic transitions are far from realized due to a lack of fundamental understanding of the atomic-scale processes that underlie migration and spatiotemporal evolution of oxygen vacancies over nano-to-mesoscopic length/timescales under applied electric field. In this project, we employ a synergistic integration of density functional theory (DFT) calculations, ab initio/classical molecular dynamics (AIMD/CMD) simulations, machine learning (ML), precision synthesis, and multi-modal X-ray imaging experiments to address this knowledge gap. Such an integrated approach offers to elucidate the correlations between subtle structural distortion and oxidation states; treat localized charge carriers; describe defect/ion transport in the presence of electric field; and, in turn, greatly advance the current understanding of microstructural evolution in complex oxides under applied bias. The fundamental knowledge gained from this work will enable precise control over hierarchical defect structures and unravel new routes to manipulate resistance states in complex oxides. This, in turn, will accelerate design of novel devices with desired set of neural functionalities, and high-speed densely-scaled resistive random access memory technologies.

36 MATERIALS SCIENCE↗

Rotational quenching of H{sub 2}O by He: Mixed quantum/classical theory and comparison with quantum results

The mixed quantum/classical theory (MQCT) formulated in the space-fixed reference frame is used to compute quenching cross sections of several rotationally excited states of water molecule by impact of He atom in a broad range of collision energies, and is tested against the full-quantum calculations on the same potential energy surface. In current implementation of MQCT method, there are two major sources of errors: one affects results at energies below 10 cm{sup −1}, while the other shows up at energies above 500 cm{sup −1}. Namely, when the collision energy E is below the state-to-state transition energy ΔE the MQCT method becomes less accurate due to its intrinsic classical approximation, although employment of the average-velocity principle (scaling of collision energy in order to satisfy microscopic reversibility) helps dramatically. At higher energies, MQCT is expected to be accurate but in current implementation, in order to make calculations computationally affordable, we had to cut off the basis set size. This can be avoided by using a more efficient body-fixed formulation of MQCT. Overall, the errors of MQCT method are within 20% of the full-quantum results almost everywhere through four-orders-of-magnitude range of collision energies, except near resonances, where the errors are somewhat larger.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Vacancy‐Enabled O3 Phase Stabilization for Manganese‐Rich Layered Sodium Cathodes

Abstract Manganese‐rich layered oxide materials hold great potential as low‐cost and high‐capacity cathodes for Na‐ion batteries. However, they usually form a P2 phase and suffer from fast capacity fade. In this work, an O3 phase sodium cathode has been developed out of a Li and Mn‐rich layered material by leveraging the creation of transition metal (TM) and oxygen vacancies and the electrochemical exchange of Na and Li. The Mn‐rich layered cathode material remains primarily O3 phase during sodiation/desodiation and can have a full sodiation capacity of ca. 220 mAh g −1 . It delivers ca. 160 mAh g −1 specific capacity between 2–3.8 V with >86 % retention over 250 cycles. The TM and oxygen vacancies pre‐formed in the sodiated material enables a reversible migration of TMs from the TM layer to the tetrahedral sites in the Na layer upon de‐sodiation and sodiation. The migration creates metastable states, leading to increased kinetic barrier that prohibits a complete O3‐P3 phase transition.

Xiao, Biwei↗

Dependence of the kinetic energy absorption capacity of bistable mechanical metamaterials on impactor mass and velocity

Using an alternative mechanism to dissipation or scattering, bistable structures and mechanical metamaterials have shown promise for mitigating the detrimental effects of impact by reversibly locking energy into strained material. Herein, we extend prior works on impact absorption via bistable metamaterials to computationally explore the dependence of kinetic energy transmission on the velocity and mass of the impactor, with strain rates exceeding 10 2 s –1 . We observe a large dependence on both impactor parameters, ranging from significantly better to worse performance than a comparative linear material. We then correlate the variability in performance to solitary wave formation in the system and give analytical estimates of idealized energy absorption capacity under dynamic loading. In addition, we find a significant dependence on damping accompanied by a qualitative difference in solitary wave propagation within the system. The complex dynamics revealed in this study offer potential future guidance for the application of bistable metamaterials to applications including human and engineered system shock and impact protection devices.

42 ENGINEERING↗

Modeling Structural Colors from Disordered One-Component Colloidal Nanoparticle-Based Supraballs Using Combined Experimental and Simulation Techniques

Bright, saturated structural colors in birds have inspired synthesis of self-assembled, disordered arrays of assembled nanoparticles with varied particle spacings and refractive indices. However, predicting colors of assembled nanoparticles, and thereby guiding their synthesis, remains challenging due to the effects of multiple scattering and strong absorption. In this work, we use a computational approach to first reconstruct the nanoparticles’ assembled structures from small-angle scattering measurements and then input the reconstructed structures to a finite-difference time-domain method to predict their color and reflectance. This computational approach is successfully validated by comparing its predictions against experimentally measured reflectance and provides a pathway for reverse engineering colloidal assemblies with desired optical and photothermal properties.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Comparison of the One-electron Oxidations of CO-Bridged vs Unbridged Bimetallic Complexes: Electron-transfer Chemistry of Os2Cp2(CO)4 and Os2Cp*2(μ-CO)2(CO)2 (Cp = η5-C5H5, Cp* = η5-C5Me5)

The one-electron oxidations of two dimers of half-sandwich osmium carbonyl complexes have been examined by electrochemistry, spectro-electrochemistry, and computational methods. The all-terminal carbonyl complex Os2Cp2(CO)4 (1, Cp = η5-C5H5) undergoes a reversible one-electron anodic reaction at E1/2 = 0.41 V vs ferrocene in CH2Cl2/0.05 M [NBu4][B(C6F5)4], giving a rare example of a metal-metal bonded radical cation unsupported by bridging ligands. The IR spectrum of 1+ is consistent with an approximately 1:1 mixture of anti and gauche structures for the 33 e- radical cation in which it has retained all-terminal bonding of the CO ligands. DFT calculations, including orbital-occupancy-perturbed Mayer bond-order analyses, show that the HOMOs of anti-1 and gauche-1 are metal-ligand delocalized. Removal of an electron from 1 has very little effect on the Os-Os bond order, accounting for the resistance of 1+ to heterolytic cleavage. The Os-Os bond distance is calculated to decrease by 0.10 Å and 0.06 Å as a consequence of one-electron oxidation of anti-1 and gauche-1, respectively. The CO-bridged complex Os2Cp*2(μ-CO)2(CO)2 (Cp* = η5-C5Me5), trans-2, undergoes a more facile oxidation, E1/2 = - 0.11 V, giving a persistent radical cation shown by solution IR analysis to preserve its bridged-carbonyl structure. However, ESR analysis of frozen solutions of 2+ is interpreted in terms of the presence of two isomers, most likely anti-2+ and trans-2+, at low temperature. Calculations show that the HOMO of trans-2 is highly delocalized over the metal-ligand framework, with the bridging carbonyls accounting for about half of the orbital makeup. The Os-Os bond order again changes very little with removal of an electron, and the Os-Os bond length actually undergoes minor shortening. Calculations suggest that the second isomer of 2+ has both the trans CO-bridged and the anti all-terminal CO structures. DRL and WEG acknowledge the support of the National Science Foundation under grant CHE-0808909. K-WH acknowledges financial support from KAUST. RMB thanks the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Biosciences and Geosciences for support. Pacific Northwest National Laboratory is a multiprogram national laboratory operated by Battelle for the U.S. Department of Energy. We thank Dr. S. I. Gorelsky for the discussion on the OOP analysis.

bonding↗

Hybrid chromophore/template nanostructures: A customizable platform material for solar energy storage and conversion

Challenges with cost, cyclability, and/or low energy density have largely prevented the development of solar thermal fuels, a potentially attractive alternative energy technology based on molecules that can capture and store solar energy as latent heat in a closed cycle. In this paper, we present a set of novel hybrid photoisomer/template solar thermal fuels that can potentially circumvent these challenges. Using first-principles computations, we demonstrate that these fuels, composed of organic photoisomers bound to inexpensive carbon-based templates, can reversibly store solar energy at densities comparable to Li-ion batteries. Furthermore, we show that variation of the template material in combination with the photoisomer can be used to optimize many of the key performance metrics of the fuel-i.e., the energy density, the storage lifetime, the temperature of the output heat, and the efficiency of the solar-to-heat conversion. Our work suggests that the solar thermal fuels concept can be translated into a practical and highly customizable energy storage and conversion technology. (C) 2013 American Institute of Physics. [http://dx.doi.org/10.1063/1.4773306]

Kolpak, AM↗

Characterisation of Al{sub 0.52}In{sub 0.48}P mesa p-i-n photodiodes for X-ray photon counting spectroscopy

Results characterising the performance of thin (2 μm i-layer) Al{sub 0.52}In{sub 0.48}P p{sup +}-i-n{sup +} mesa photodiodes for X-ray photon counting spectroscopy are reported at room temperature. Two 200 μm diameter and two 400 μm diameter Al{sub 0.52}In{sub 0.48}P p{sup +}-i-n{sup +} mesa photodiodes were studied. Dark current results as a function of applied reverse bias are shown; dark current densities <3 nA/cm{sup 2} were observed at 30 V (150 kV/cm) for all the devices analysed. Capacitance measurements as a function of applied reverse bias are also reported. X-ray spectra were collected using 10 μs shaping time, with the device illuminated by an {sup 55}Fe radioisotope X-ray source. Experimental results showed that the best energy resolution (FWHM) achieved at 5.9 keV was 930 eV for the 200 μm Al{sub 0.52}In{sub 0.48}P diameter devices, when reverse biased at 15 V. System noise analysis was also carried out, and the different noise contributions were computed.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Structural Studies of Amorphous Materials by Fluctuation Electron Microscopy

Fluctuation Electron Microscopy (FEM) is a technique that examines the fluctuations in electron scattering across a uniformly thin amorphous sample. The statistics of the intensity fluctuations, mean and variance, reveal any underlying medium-range order present in the structure. The goals of this project were: (1) To determine the fundamentals of the scattering physics that gives rise to the variance signal in fluctuation electron microscopy (FEM); (2) To use these discoveries to find ways to quantify FEM; (3) To apply the FEM method to interesting and technologically important families of amorphous materials, particularly those with important applications in energy-related processes. Excellent progress was made in items (1) and (2). In stage (3) we did not examine the metamict zircons, as proposed. Instead, we examined films of polycrystalline and amorphous semi-conducting diamond. Significant accomplishments are: (1) A Reverse Monte Carlo procedure was successfully implemented to invert FEM data into a structural model. This is computer-intensive, but it demonstrated that diffraction and FEM data from amorphous silicon are most consistent with a paracrystallite model. This means that there is more diamond-like topology present in amorphous silicon than is predicted by the continuous random network model. (2) There is significant displacement decoherence arising in diffraction from amorphous silicon and carbon. The samples are being bombarded by the electron beam and atoms do not stay still while being irradiated – much more than was formerly understood. The atom motions cause the destructive and constructive interferences in the diffraction pattern to fluctuate with time, and it is the time-averaged speckle that is being measured. The variance is reduced by a factor m, 4 ≤ m ≤ 1000, relative to that predicted by kinematical scattering theory. (3) Speckle intensity obeys a gamma distribution, where the mean intensity $ \overline{I}\ $ and m are the two parameters governing the shape of the gamma distribution profile. m is determined by the illumination spatial coherence, which is normally very high, and mostly by the displacement decoherence within the sample. (4) Amorphous materials are more affected by the electron beam than are crystalline materials. Different samples exhibit different disruptibility, as measured by the effective values of m that fit the data. (5) Understanding the origin of the displacement decoherence better should lead to efficient methods for computing the observed variance from amorphous materials.

36 MATERIALS SCIENCE↗

Low-rank factorization of electron integral tensors and its application in electronic structure theory

In this letter, we introduce the reverse Cuthill-McKee (RCM) algorithm, which is often used for the bandwidth reduction of sparse tensors, to transform the two-electron integral tensors to their block diagonal forms. By further applying the pivoted Cholesky decomposition (CD) on each of the diagonal blocks, we are able to represent the high-dimensional two-electron integral tensors in terms of permutation matrices and low-rank Cholesky vectors. This representation facilitates the low-rank factorization of the high-dimensional tensor contractions that are usually encountered in post-Hartree-Fock calculations. In this letter, we discuss the second-order Møller-Plesset (MP2) method and linear coupled- cluster model with doubles (L-CCD) as two simple examples to demonstrate the efficiency of the RCM-CD technique in representing two-electron integrals in a compact form.

electronic structure theory↗

Ultrasonic imaging in liquid sodium

The fourth generation of nuclear reactor can use liquid sodium as the core coolant. When the reactor is operating, sodium temperatures can reach up to 600 deg. C. During maintenance periods, when the reactor is shut down, the coolant temperature is reduced to 200 deg. C. Because molten sodium is optically opaque, ultrasonic imaging techniques are developed for maintenance activities. Under-sodium imaging aims at i) checking the health of immersed structures. It should also allow ii) to assess component degradation or damage as cracks and shape defects as well as iii) the detection of lost objects. The under-sodium imaging system has to sustain high temperature (up to 300 deg. C) and hostility of the sodium environment. Furthermore, specific constraints such as transducers characteristics or the limited sensor mobility in the reactor vessel have to be considered. This work focuses on developing a methodology for detecting damages such as crack defects with ultrasound devices. Surface-breaking cracks or deep cracks are sought in the weld area, as welds are more subject to defects. Traditional methods enabled us to detect emerging cracks of submillimeter size with sodium-compatible high-temperature transducer. The presented approach relies on making use of prior knowledge about the environment through the implementation of differential imaging and time-reversal techniques. Indeed, this approach allows to detect a change by comparison with a reference measurement and by focusing back to any change in the environment. It is a means of analysis and understanding of the physical phenomena making it possible to design more effective inspection strategies. Difference between the measured signals reveals the acoustic field scattered by a perturbation (a crack for instance), which may occur between periodical measurements. The imaging method relies on the adequate combination of two computed ultrasonic fields, one forward and one adjoint. The adjoint field, which carries the information about the defects, is analogous to a time-reversal operation. One of the interests of the presented method is that the time-reversal operation is not done experimentally but numerically. Numerical simulations have been carried out to validate the practical relevance of this approach. The preliminary numerical results show a nice agreement between the guessed and the actual positions of the defect. After water-tests, in sodium-tests must be done in order to validate the water/sodium transposition. For this purpose, an under-sodium device is under development, which can move the transducers with four degrees of freedom in a 1.5 m{sup 3} sodium pot. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

A unified thermionic and thermionic-field emission (TE–TFE) model for ideal Schottky reverse-bias leakage current

We present a unified thermionic emission (TE) and thermionic-field emission (TFE) model for the ideal reverse-bias leakage current in Schottky junctions. The unified TE–TFE analytical model advances upon previous analytical TFE models by Murphy–Good and Padovani–Stratton, which are the two most widely adopted models by the community, in two major aspects: (i) the applicability of the TFE expression therein is extended to near-zero surface electric fields by an error-function correction, allowing for the calculation of the total current by a nontrivial sum of TE (over-the-barrier current) and TFE (below-the-barrier current) contributions; therefore, an accurate description of the TE-to-TFE transition region is captured analytically for the first time; (ii) image-force lowering is considered with much-simpler correction terms. Comparisons with the reference numerical model show that the unified TE–TFE model has excellent accuracy, as well as a 10 000× reduction in computation time. The unified model is further tested against experimental data from Schottky barrier diodes based on Si, 4H-SiC, GaN, and β-Ga 2 O 3 , revealing accurate extractions of barrier heights and correct descriptions of the ideal reverse leakage characteristics. With the extended applicable range, improved accuracy, and computational efficiency, the unified TE–TFE model is highly valuable for the design and analysis of devices based on Schottky junctions, as well as for potential integration in technology computer-aided design (TCAD) tools.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

High–Energy Earth–Abundant Cathodes with Enhanced Cationic/Anionic Redox for Sustainable and Long–Lasting Na–Ion Batteries

Layered iron/manganese-based oxides are a class of promising cathode materials for sustainable batteries due to their high energy densities and earth abundance. However, the stabilization of cationic and anionic redox reactions in these cathodes during cycling at high voltage remain elusive. Here, an electrochemically/thermally stable P2-Na 0.67 Fe 0.3 Mn 0.5 Mg 0.1 Ti 0.1 O 2 cathode material with zero critical elements is designed for sodium-ion batteries (NIBs) to realize a highly reversible capacity of ≈210 mAh g –1 at 20 mA g –1 and good cycling stability with a capacity retention of 74% after 300 cycles at 200 mA g –1 , even when operated with a high charge cut-off voltage of 4.5 V versus sodium metal. Combining a suite of cutting-edge characterizations and computational modeling, it is shown that Mg/Ti co-doping leads to stabilized surface/bulk structure at high voltage and high temperature, and more importantly, enhances cationic/anionic redox reaction reversibility over extended cycles with the suppression of other undesired oxygen activities. This work fundamentally deepens the failure mechanism of Fe/Mn-based layered cathodes and highlights the importance of dopant engineering to achieve high-energy and earth-abundant cathode material for sustainable and long-lasting NIBs.

25 ENERGY STORAGE↗

Qualitative and quantitative enhancement of parameter estimation for model-based diagnostics using automatic differentiation with an application to inertial fusion

Parameter estimation using observables is a fundamental concept in the experimental sciences. Mathematical models that represent the physical processes can enable reconstructions of the experimental observables and greatly assist in parameter estimation by turning it into an optimization problem which can be solved by gradient-free or gradient-based methods. In this work, the recent rise in flexible frameworks for developing differentiable scientific computing programs is leveraged in order to dramatically accelerate data analysis of a common experimental diagnostic relevant to laser–plasma and inertial fusion experiments, Thomson scattering. A differentiable Thomson-scattering data analysis tool is developed that uses reverse-mode automatic differentiation (AD) to calculate gradients. By switching from finite differencing to reverse-mode AD, three distinct outcomes are achieved. First, gradient descent is accelerated dramatically to the extent that it enables near real-time usage in laser–plasma experiments. Second, qualitatively novel quantities which require $\mathcal{O}(10^3)$ parameters can now be included in the analysis of data which enables unprecedented measurements of small-scale laser–plasma phenomena. Third, uncertainty estimation approaches that leverage the value of the Hessian become accurate and efficient because reverse-mode AD can be used for calculating the Hessian.

97 MATHEMATICS AND COMPUTING↗

Dual-ion ECRAM as a stable and accurate analog synapse

Electrochemical random-access memory (ECRAM) works by tuning the bulk electronic conductance of functional materials via reversible, electrochemical insertion of ions, resulting in stable analog resistive switching, attractive for analog in-memory and neuromorphic computing. However, achieving fast programming for training and long retention for inference has been elusive. Protonic ECRAM demonstrates fast programming but insufficient retention, while oxygen-based ECRAM with excellent retention requires elevated programming temperatures. Cu-based ECRAM offers a compromise, with an activation energy (E A ) of ≈0.76 eV between protons (E A ≈ 0.4 eV) and oxygen (E A > 1 eV), enabling extensive retention and room temperature programming. Combining Cu 2+ ions with protons to form a dual-ion ECRAM, we demonstrate two distinct switching behaviors: fast switching at ≤5 V, (E A ≈ 0.45 eV) via protons, and nonvolatile, room temperature switching at ≥8 V, with E A ≈ 0.76 eV via Cu 2+ ions. In conclusion, the Cu-based state exhibits a wide conductance range, with excellent retention, low noise, and linear current-voltage behavior, achieving digital-equivalent ImageNet inference accuracy.

analog in-memory computing↗

A high-temperature ferromagnetic topological insulating phase by proximity coupling

Topological insulators are insulating materials that display conducting surface states protected by time-reversal symmetry 1 , 2 , wherein electron spins are locked to their momentum. This unique property opens up new opportunities for creating next-generation electronic, spintronic and quantum computation devices 3 , 4 , 5 . Introducing ferromagnetic order into a topological insulator system without compromising its distinctive quantum coherent features could lead to the realization of several predicted physical phenomena 6 , 7 . In particular, achieving robust long-range magnetic order at the surface of the topological insulator at specific locations without introducing spin-scattering centres could open up new possibilities for devices. Here we use spin-polarized neutron reflectivity experiments to demonstrate topologically enhanced interface magnetism by coupling a ferromagnetic insulator (EuS) to a topological insulator (Bi 2 Se 3 ) in a bilayer system. This interfacial ferromagnetism persists up to room temperature, even though the ferromagnetic insulator is known to order ferromagnetically only at low temperatures (<17 K). The magnetism induced at the interface resulting from the large spin–orbit interaction and the spin–momentum locking of the topological insulator surface greatly enhances the magnetic ordering (Curie) temperature of this bilayer system. The ferromagnetism extends ~2 nm into the Bi 2 Se 3 from the interface. Owing to the short-range nature of the ferromagnetic exchange interaction, the time-reversal symmetry is broken only near the surface of a topological insulator, while leaving its bulk states unaffected. The topological magneto-electric response originating in such an engineered topological insulator 2 , 8 could allow efficient manipulation of the magnetization dynamics by an electric field, providing an energy-efficient topological control mechanism for future spin-based technologies

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗