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At least 55 records · Page 3

Reversible migration of silver on memorized pathways in Ag-Ge{sub 40}S{sub 60} films

Reversible and reproducible formation and dissolution of silver conductive filaments are studied in Ag-photodoped thin-film Ge{sub 40}S{sub 60} subjected to electric fields. A tip-planar geometry is employed, where a conductive-atomic-force microscopy tip is the tip electrode and a silver patch is the planar electrode. We highlight an inherent “memory” effect in the amorphous chalcogenide solid-state electrolyte, in which particular silver-ion migration pathways are preserved “memorized” during writing and erasing cycles. The “memorized” pathways reflect structural changes in the photodoped chalcogenide film. Structural changes due to silver photodoping, and electrically-induced structural changes arising from silver migration, are elucidated using Raman spectroscopy. Conductive filament formation, dissolution, and electron (reduction) efficiency in a lateral device geometry are related to operation of the nano-ionic Programmable Metallization Cell memory and to newly emerging chalcogenide-based lateral geometry MEMS technologies. The methods in this work can also be used for qualitative multi-parameter sampling of metal/amorphous-chalcogenide combinations, characterizing the growth/dissolution rates, retention and endurance of fractal conductive filaments, with the aim of optimizing devices.

36 MATERIALS SCIENCE↗

DEVELOPMENT OF INEXPENSIVE HIGH TEMPERATURE NITI-BASED SHAPE MEMORY ALLOYS FOR POWDER BED ADDITIVE MANUFACTURING

NiTi and NiTi-based Shape Memory Alloys (SMA) exhibit a reversible solid-state phase transformation from martensite to austenite driven by thermal energy. High temperature (Mf>100°C) SMAs are martensite at room temperature and can be fabricated into solid-state actuators that return to a pre-programmed shape against a designed load after heating to transformation threshold. Reactive as-fabricated additively manufactured parts (4-D printing) is the current state of the art in manufacturing of SMAs but requires compositions compliant to rapid solidification. Existing actuator designs are developed from commercially available, highly investigated material compositions. However, existing high temperature high performance (high actuation strain, low thermal hysteresis) shape memory alloys contain significant (>10% at.) portions of high-cost Platinum Group Metals (PGMs). It is of significant scientific interest to investigate material compositions that are peer performing or superior to PGMs whose constituent elements represent a significant cost savings. Shape memory alloy properties vary significantly with small (0.1% at.) compositional changes making robust investigative sample sets very large. Computational material design can be deployed to shrink the compositional space of possible alloy combinations and reduce the experimental load in material discovery. Investigating shape memory effect (SME) and validating process additive process parameters for a single novel composition is cost intensive in both time and consumed materials. Additionally, sub-optimal processing, oxygen, or solidification rate sensitivity could render additively manufacturing specimens without micro, macro cracks, or significant chemical variance impossible. Unfortunately, such failure susceptibility cannot be simulated. Therefore, a research pathway to validate novel shape memory alloy compositions for powder bed fusion additive manufacturing without the need for powdered feedstock is also proposed. This research investigates novel high temperature shape memory alloys for actuators without platinum group alloying elements to discover one that could be commercially viable as an additive manufacturing feedstock.

Sundermann, Tayler↗

Electrochemical Random-Access Memory: Progress, Perspectives, and Opportunities

Non-von Neumann computing using neuromorphic systems based on analogue synaptic and neuronal elements has emerged as a potential solution to tackle the growing need for more efficient data processing, but progress toward practical systems has been stymied due to a lack of materials and devices with the appropriate attributes. Recently, solid state electrochemical ion-insertion, also known as electrochemical random access memory (ECRAM) has emerged as a promising approach to realize the needed device characteristics. ECRAM is a three terminal device that operates by tuning electronic conductance in functional materials through solid-state electrochemical redox reactions. This mechanism can be considered as a gate-controlled bulk modulation of dopants and/or phases in the channel. Early work demonstrating that ECRAM can achieve nearly ideal analogue synaptic characteristics has sparked tremendous interest in this approach. More recently, the realization that electrochemical ion insertion can be used to tune the electronic properties of many types of materials including transition metal oxides, layered two-dimensional materials, organic and coordination polymers, and that the changes in conductance can span orders of magnitude has further attracted interest in ECRAM as the basis for analogue synaptic elements for inference accelerators as well as for dynamical devices that can emulate a wide range of neuronal characteristics for implementation in analogue spiking neural networks. At its core, ECRAM shares many fundamental aspects with rechargeable batteries, where ion insertion materials are used extensively for their ability to reversibly store charge and energy. Computing applications, however, present drastically different requirements: systems will require many millions of devices, scaled down to tens of nanometers, all while achieving reliable electronic-state tuning at scaled-up rates and endurances, and with minimal energy dissipation and noise. Further, in this review, we discuss the history, basic concepts, recent progress, as well as the challenges and opportunities for different types of ECRAM, broadly grouped by their primary mobile ionic charge carrier, including Li, protons, and oxygen vacancies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Well Monitoring System For EGS

This grant is a collection of projects designed to move aircraft high temperature electronics technology into the geothermal industry. Randy Normann is the lead. He licensed the HT83SNL00 chip from Sandia National Labs. This chip enables aircraft developed electronics for work within a geothermal well logging tool. However, additional elements are needed to achieve commercially successful logging tools. These elements are offered by a strong list of industrial partners on this grant as: Electrochemical Systems Inc. for HT Rechargeable Batteries, Frequency Management Systems for 300C digital clock, Sandia National Labs for experts in high temperature solder, Honeywell Solid-State Electronics Center for reprogrammable high temperature memory. During the course of this project MagiQ Technologies for high temperature fiber optics.

15 GEOTHERMAL ENERGY↗

Shape-memory transformations of NiTi: Minimum-energy pathways between austenite, martensites, and kinetically limited intermediate states

NiTi is the most used shape-memory alloy, nonetheless, a lack of understanding remains regarding the associated structures and transitions, including their barriers. Using a generalized solid-state nudge elastic band (GSSNEB) method implemented via density-functional theory, we detail the structural transformations in NiTi relevant to shape memory: those between body-centered orthorhombic (BCO) groundstate and a newly identified stable austenite (“glassy” B2-like) structure, including energy barriers (hysteresis) and intermediate structures (observed as a kinetically limited R-phase), and between martensite variants (BCO orientations). All results are in good agreement with available experiment. We contrast the austenite results to those from the often-assumed, but unstable B2. Furthermore, these high- and low-temperature structures and structural transformations provide much needed atomic-scale detail for transitions responsible for NiTi shape-memory effects.

36 MATERIALS SCIENCE↗

Maximizing dynamic range and performance of anatase TiO 2 ECRAM through structure and programming

Here, in this study, we investigate the structure-dependent modulation characteristics of all-solid-state three-terminal electrochemical random-access memory (ECRAM) based on an anatase Li x TiO 2 channel. By directly comparing “asymmetric” and “symmetric” ECRAM device architectures, we reveal significant insight into the impact of a non-zero gate-drain open-circuit voltage and its influence on voltage vs. current-controlled gating. We also explore the impact of potentiation/depression write parameters on the symmetry, linearity, and dynamic range of the device response. Together, initial results from optimizing structure and programming approaches yielded unprecedented G max /G min ratios of >1,000 for ECRAM and hundreds of tunable memory states with excellent linearity and symmetry. Simulations based on these ECRAM devices further illustrate the promise of this analog memory technology, achieving near 2% classification error in the MNIST digit recognition benchmark for a range of training parameters compared to a theoretical best of 1.66% and outperforming other device models extracted from the literature.

AIHWKit↗

Observation of 0–π transition in SIsFS Josephson junctions

The 0–π transition in Superconductor-Insulator-superconductor-Ferromagnet-Superconductor (SIsFS) Josephson junctions (JJs) was investigated experimentally. As predicted by theory, an s-layer inserted into a ferromagnetic SIFS junction can enhance the critical current density up to the value of an SIS tunnel junction. We fabricated Nb′ | AlO{sub x} | Nb | Ni{sub 60}Cu{sub 40} | Nb JJs with wedge-like s (Nb) and F (Ni{sub 60}Cu{sub 40}) layers and studied the Josephson effect as a function of the s- and F-layer thickness, d{sub s} and d{sub F}, respectively. For d{sub s} = 11 nm, π-JJs with SIFS-type j{sub c}(d{sub F}) and critical current densities up to j{sub c}{sup π}=60 A/cm{sup 2} were obtained at 4.2 K. Thicker d{sub s} led to a drastic increase of the critical current decay length, accompanied by the unexpected disappearance of the 0–π transition dip in the j{sub c}(d{sub F}) dependence. Our results are relevant for superconducting memories, rapid single flux quantum logic circuits, and solid state qubits.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Strongly correlated perovskite lithium ion shuttles

Solid-state ion shuttles are of broad interest in electrochemical devices, nonvolatile memory, neuromorphic computing, and biomimicry utilizing synthetic membranes. Traditional design approaches are primarily based on substitutional doping of dissimilar valent cations in a solid lattice, which has inherent limits on dopant concentration and thereby ionic conductivity. Here, we demonstrate perovskite nickelates as Li-ion shuttles with simultaneous suppression of electronic transport via Mott transition. Electrochemically lithiated SmNiO 3 (Li-SNO) contains a large amount of mobile Li + located in interstitial sites of the perovskite approaching one dopant ion per unit cell. A significant lattice expansion associated with interstitial doping allows for fast Li + conduction with reduced activation energy. We further present a generalization of this approach with results on other rare-earth perovskite nickelates as well as dopants such as Na + . The results highlight the potential of quantum materials and emergent physics in design of ion conductors.

36 MATERIALS SCIENCE↗

Charge trapping properties of Ge nanocrystals grown via solid-state dewetting

In the present work, we report on the charge trapping properties of Germanium Nanocrystals (Ge NCs) self assembled on SiO 2 thin layer for promising applications in next-generation non volatile memory by the means of Deep Level Transient Spectroscopy (DLTS) and high frequency C-V method. The Ge NCs were grown via dewetting phenomenon at solid state by Ultra-High Vacuum (UHV) annealing and passivated with silicon before SiO 2 capping. The role of the surface passivation is to reduce the electrical defect density at the Ge NCs-SiO 2 interface. The presence of the Ge NCs in the oxide of the MOS capacitors strongly affects the C-V characteristics and increases the accumulation capacitance, causes a negative flat band voltage (VFB) shift. The DLTS has been used to study the individual Ge NCs as a single point deep level defect in the oxide. DLTS reveals two main features: the first electron traps around 255 K could correspond to dangling bonds at the Si/SiO2 interface and the second, at high-temperature (>300 K) response, could be originated from minority carrier generation in Ge NCs.

36 MATERIALS SCIENCE↗

Large room-temperature elastocaloric effect in a bulk polycrystalline Ni-Ti-Cu-Co alloy with low isothermal stress hysteresis

Creation of high-performance advanced elastocaloric materials is essential for the execution of elastocaloric refrigeration that can be an environment-friendly and high-efficiency substitute for the widely used traditional vapor-compression cooling technology. Here we have developed a bulk polycrystalline Ni-Ti-Cu-Co shape memory alloy exhibiting large elastocaloric effect, low stress hysteresis and room temperature working temperature, all of which are of great importance to and urgently demanded for high-efficiency room-temperature elastocaloric refrigeration. This newly developed (Ni 42.5 Ti 50 Cu 7.5 ) 99 Co 1 alloy shows a large room-temperature elastocaloric effect with directly measured adiabatic temperature change up to -14.4 K during unloading. The stress hysteresis of the isothermal superelastic stress-strain curve is as low as 60 MPa when the maximum tensile strain is 2.7%. Owing to the large elastocaloric effect and low stress hysteresis, a very high coefficient of performance up to 19 is achieved on the material level. This newly developed (Ni 42.5 Ti 50 Cu 7.5 ) 99 Co 1 alloy is a robust candidate for efficient elastocaloric refrigeration. Advanced in-situ synchrotron high-energy X-ray diffraction technique was employed to reveal the phase transformation sequence and to accurately determine the crystal structure of different phases, based on which the lattice compatibility between the transforming phases was evaluated and the phase transformation strain was predicted, providing in-depth fundamental understanding of the martensitic transformation in this newly developed alloy. This work could be useful for designing high-performance elastocaloric materials for solid-state cooling applications.

36 MATERIALS SCIENCE↗

Endowing low fatigue for elastocaloric effect by refined hierarchical microcomposite in additive manufactured NiTiCuCo alloy

Abstract NiTiCu-based shape memory alloys have been considered as ideal materials for solid-state refrigeration due to their superb cycling stability for elastocaloric effect. However, the embrittlement and deterioration caused by secondary phase and coarse grains restrict their applications, and it is still challenging since the geometric components are required. Here, bulk NiTiCuCo parts with excellent forming quality were fabricated by laser powder bed fusion (LPBF) technique. The as-fabricated alloy exhibits refined three-phases hierarchical microcomposite formed based on the rapid cooling mode of LPBF, composed of intricate dendritic Ti 2 Ni–NiTi composite and nano Ti 2 Cu embedded inside the NiTi-matrix. This configuration endows far superior elastocaloric stability compared to the as-cast counterpart. The low fatigue stems from the strong elastic coupling between the interphases with reversible martensite transformation, revealed byin-situsynchrotron high-energy x-ray diffraction. The fabrication of NiTiCuCo alloy via LPBF fills the bill of complex geometric structures for elastocaloric NiTiCu alloys. The understanding of interphase micro-coupling could provide the guide for designing LPBF fabricated shape memory-based composites, enabling their applications for special demands on other functionalities.

Engineering↗

Lattice Vibrations Boost Demagnetization Entropy in Shape Memory Alloy

Magnetocaloric (MC) materials present an avenue for chemical-free, solid state refrigeration through cooling via adiabatic demagnetization. We have used inelastic neutron scattering to measure the lattice dynamics in the MC material Ni 45 Co 5 Mn 36.6 In 13.4 . Upon heating across TC, the material exhibits an anomalous increase in phonon entropy of 0.17 0.04 k_B/atom, which is nine times larger than expected from conventional thermal expansion. We find that the phonon softening is focused in a transverse optic phonon, and we present the results of first-principle calculations which predict a strong coupling between lattice distortions and magnetic excitations.

36 MATERIALS SCIENCE↗

Electrical probing of field-driven cascading quantized transitions of skyrmion cluster states in MnSi nanowires

Magnetic skyrmions are topologically stable whirlpool-like spin textures that offer great promise as information carriers for future spintronic devices. To enable such applications, particular attention has been focused on the properties of skyrmions in highly confined geometries such as one-dimensional nanowires. Hitherto, it is still experimentally unclear what happens when the width of the nanowire is comparable to that of a single skyrmion. Here, we achieve this by measuring the magnetoresistance in ultra-narrow MnSi nanowires. We observe quantized jumps in magnetoresistance versus magnetic field curves. By tracking the size dependence of the jump number, we infer that skyrmions are assembled into cluster states with a tunable number of skyrmions, in agreement with the Monte Carlo simulations. Our results enable an electric reading of the number of skyrmions in the cluster states, thus laying a solid foundation to realize skyrmion-based memory devices.

36 MATERIALS SCIENCE↗

All-optical reconfiguration of single silicon-vacancy centers in diamond for non-volatile memories

Strain engineering is vital for tuning the optical and spin properties of solid-state color centers, enhancing spin coherence and compensating emission wavelength shift. Here, we develop an all-optical approach to directly modify the local strain of color centers at the nanoscale by migrating the nearby defect. High-power pulsed optical irradiation triggers defect migration, which subsequently leads to the redistribution of the local crystal lattice of the host material. This redistribution alters the strain experienced by nearby color centers. Using silicon-vacancy centers in diamond, we validate this method and demonstrate a ground state splitting enhancement of up to 1.8 THz. Unlike conventional methods, our approach requires no external fields or nanostructure modifications, enabling non-volatile strain control and optical memory functionality across wide temperature ranges. Its local, permanent nature offers a scalable path for enhancing spin coherence in large-scale quantum systems and has potential applications in photonic machine learning.

Nanoscale devices↗

Magneto-ionic control of magnetism using a solid-state proton pump

Voltage-gated ion transport as a means of manipulating magnetism electrically could enable ultralow-power memory, logic and sensor technologies. Earlier work made use of electric-field-driven O 2– displacement to modulate magnetism in thin films by controlling interfacial or bulk oxidation states. However, elevated temperatures are required and chemical and structural changes lead to irreversibility and device degradation. Here we show reversible and non-destructive toggling of magnetic anisotropy at room temperature using a small gate voltage through H + pumping in all-solid-state heterostructures. We achieve 90° magnetization switching by H + insertion at a Co/GdO x interface, with no degradation in magnetic properties after >2,000 cycles. We then demonstrate reversible anisotropy gating by hydrogen loading in Pd/Co/Pd heterostructures, making metal–metal interfaces susceptible to voltage control. The hydrogen storage metals Pd and Pt are high spin–orbit coupling materials commonly used to generate perpendicular magnetic anisotropy, Dzyaloshinskii–Moriya interaction, and spin–orbit torques in ferromagnet/heavy-metal heterostructures. Furthermore, our work provides a platform for voltage-controlled spin–orbitronics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Simultaneously achieved large reversible elastocaloric and magnetocaloric effects and their coupling in a magnetic shape memory alloy

Large reversible caloric effects covering a broad temperature region are essential for high-efficiency and environment-friendly solid-state caloric refrigeration that can potentially replace the traditional vaporcompression-based cooling technology. Here, we report the simultaneously achieved large reversible magnetocaloric and elastocaloric effects in a Ni 43 Co 6 Mn 40 Sn 11 magnetic shape memory alloy. A reversible near-room-temperature magnetic entropy change Δ S m of as high as 19.3 J kg –1 K –1 under 5 T was experimentally obtained and the corresponding adiabatic temperature change Δ T ad was estimated to be 7.7 K. Meanwhile, a large reversible elastocaloric effect with a directly measured Δ T ad up to 7.1 K was attained. The elastocaloric effect exhibits high cyclic stability with no apparent degradation during 380 cycles of loading and unloading. Furthermore, we propose and demonstrate the utilization of the multicaloric approach under the coupled uniaxial stress and magnetic field to enlarge the refrigeration temperature region of reversible caloric effects. By combining the reversible magnetocaloric and elastocaloric effects and the reversible multicaloric effect under the coupling of uniaxial stress and magnetic field in the hysteresis region, large reversible caloric effects covering a broad temperature region from 257 K to 383 K can be obtained. Finally, this study may pave the way for designing advanced caloric materials with cyclically stable and reversible large caloric effects and wide refrigeration temperature region for solid-state refrigeration.

36 MATERIALS SCIENCE↗

Microstructure and transformation behavior of Ni{sub 24.7}Ti{sub 50.3}Pd{sub 25} high temperature shape-memory alloy with Sc micro-addition

NiTiPd shape-memory alloys (SMAs) are potential functional materials for use as solid-state actuators in the temperature range 100–250 °C. The present study investigates the effect of 1.0 at.% Sc micro-addition to Ni{sub 24.7}Ti{sub 50.3}Pd{sub 25} alloy, Sc replacing either Ti or Ni. Results show that all the three alloys studied have stable transformation behavior on stress-free thermal cycling and hence, are suitable for cyclic actuation applications. However, the addition of Sc to NiTiPd alloy leads to decrease of transformation temperatures, the magnitude of decrease being greater for the alloy with Sc replacing Ni. The martensite finish (M{sub f}) temperature of 181 °C for the NiTiPd alloy decreased to 139 °C for Sc replacing Ti and 83 °C for Sc replacing Ni. Also, the indentation modulus of NiTiPdSc (Sc replacing Ni) alloy is found to be significantly low compared to the other alloys. Analysis indicates that the observed differences in the alloy properties are related to the solubility of Sc in the NiTiPd matrix. While the quaternary NiTiPdSc alloy, Sc replacing Ti, has a single phase microstructure, the alloy with Sc replacing Ni shows the presence of Sc-rich and TiPd-type second phases in the microstructure. TEM examination revealed that the TiPd-type phase has a distinct rod-like morphology (30–50 nm) arranged in a grid-like structure. The transformation and indentation behavior of the alloys is elucidated using thermodynamic calculations of frictional energy and an electronic structure based analysis. - Highlights: • TEM of Ni{sub 23.7}Ti{sub 50.3}Pd{sub 25}Sc{sub 1} showed distinct grid of TiPd-type phase nanorods < 50 nm. • Stress-free thermal cycling of all the three alloys showed stable transformation behavior. • Ni{sub 24.7}Ti{sub 49.3}Pd{sub 25}Sc{sub 1} and Ni{sub 23.7}Ti{sub 50.3}Pd{sub 25}Sc{sub 1} showed single and multiphase structures. • Sc micro-addition (1 at.%) to Ni{sub 24.7}Ti{sub 50.3}Pd{sub 25} alloy decreased TTs significantly. • Ni{sub 23.7}Ti{sub 50.3}Pd{sub 25}Sc{sub 1} exhibited lower modulus of 67 GPa to 85 GPa of Ni{sub 24.7}Ti{sub 50.3}Pd{sub 25}.

36 MATERIALS SCIENCE↗

Strong spin–orbit quenching via the product Jahn–Teller effect in neutral group IV qubits in diamond

Abstract Artificial atom qubits in diamond have emerged as leading candidates for a range of solid-state quantum systems, from quantum sensors to repeater nodes in memory-enhanced quantum communication. Inversion-symmetric group IV vacancy centers, comprised of Si, Ge, Sn, and Pb dopants, hold particular promise as their neutrally charged electronic configuration results in a ground-state spin triplet, enabling long spin coherence above cryogenic temperatures. However, despite the tremendous interest in these defects, a theoretical understanding of the electronic and spin structure of these centers remains elusive. In this context, we predict the ground-state and excited-state properties of the neutral group IV color centers from first principles. We capture the product Jahn–Teller effect found in the excited state manifold to second order in electron–phonon coupling, and present a nonperturbative treatment of the effect of spin–orbit coupling. Importantly, we find that spin–orbit splitting is strongly quenched due to the dominant Jahn–Teller effect, with the lowest optically-active 3 E u state weakly split into m s -resolved states. The predicted complex vibronic spectra of the neutral group IV color centers are essential for their experimental identification and have key implications for use of these systems in quantum information science.

Materials Science↗