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At least 775 records · Page 43

Ionic field effect and memristive phenomena in single-point ferroelectric domain switching

Electric field induced polarization switching underpins most functional applications of ferroelectric materials in information technology, materials science, and optoelectronics. In the last 20 years, much attention has been focused on the switching of individual domains using scanning probe microscopy, both as model of ferroelectric data storage and approach to explore fundamental physics of ferroelectric switching. The classical picture of tip induced switching includes formation of cylindrical domain oriented along the tip field, with the domain size is largely determined by the tip-induced field distribution and domain wall motion kinetics. The polarization screening is recognized as a necessary precondition to the stability of ferroelectric phase; however, screening processes are generally considered to be uniformly efficient and not leading to changes in switching behavior. Here, we demonstrate that single-point tip-induced polarization switching can give rise to a surprisingly broad range of domain morphologies, including radial and angular instabilities. These behaviors are traced to the surface screening charge dynamics, which in some cases can even give rise to anomalous switching against the electric field (ionic field effect). The implications of these behaviors for ferroelectric materials and devices are discussed.

Ievlev, Anton↗

Simultaneous observation of the quantization and the interference pattern of a plasmonic near-field

Surface plasmon polaritons can confine electromagnetic fields in subwavelength spaces and are of interest for photonics, optical data storage devices and biosensing applications. In analogy to photons, they exhibit wave–particle duality, whose different aspects have recently been observed in separate tailored experiments. Here we demonstrate the ability of ultrafast transmission electron microscopy to simultaneously image both the spatial interference and the quantization of such confined plasmonic fields. Our experiments are accomplished by spatiotemporally overlapping electron and light pulses on a single nanowire suspended on a graphene film. The resulting energy exchange between single electrons and the quanta of the photoinduced near-field is imaged synchronously with its spatial interference pattern. In conclusion, this methodology enables the control and visualization of plasmonic fields at the nanoscale, providing a promising tool for understanding the fundamental properties of confined electromagnetic fields and the development of advanced photonic circuits.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Magnetization-polarization cross-control near room temperature in hexaferrite single crystals

Mutual control of the electricity and magnetism in terms of magnetic (H) and electric (E) fields, the magnetoelectric (ME) effect, offers versatile low power consumption alternatives to current data storage, logic gate, and spintronic devices. Despite its importance, E-field control over magnetization (M) with significant magnitude was observed only at low temperatures. Here we have successfully stabilized a simultaneously ferrimagnetic and ferroelectric phase in a Y-type hexaferrite single crystal up to 450 K, and demonstrated the reversal of large non-volatile M by E field close to room temperature. Manipulation of the magnetic domains by E field is directly visualized at room temperature by using magnetic force microscopy. The present achievement provides an important step towards the application of ME multiferroics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Metaplastic and energy-efficient biocompatible graphene artificial synaptic transistors for enhanced accuracy neuromorphic computing

CMOS-based computing systems that employ the von Neumann architecture are relatively limited when it comes to parallel data storage and processing. In contrast, the human brain is a living computational signal processing unit that operates with extreme parallelism and energy efficiency. Although numerous neuromorphic electronic devices have emerged in the last decade, most of them are rigid or contain materials that are toxic to biological systems. In this work, we report on biocompatible bilayer graphene-based artificial synaptic transistors (BLAST) capable of mimicking synaptic behavior. The BLAST devices leverage a dry ion-selective membrane, enabling long-term potentiation, with ~50 aJ/µm 2 switching energy efficiency, at least an order of magnitude lower than previous reports on two-dimensional material-based artificial synapses. The devices show unique metaplasticity, a useful feature for generalizable deep neural networks, and we demonstrate that metaplastic BLASTs outperform ideal linear synapses in classic image classification tasks. With switching energy well below the 1 fJ energy estimated per biological synapse, the proposed devices are powerful candidates for bio-interfaced online learning, bridging the gap between artificial and biological neural networks.

97 MATHEMATICS AND COMPUTING↗

Electric-field control of the nucleation and motion of isolated three-fold polar vertices

Recently various topological polar structures have been discovered in oxide thin films. Despite the increasing evidence of their switchability under electrical and/or mechanical fields, the dynamic property of isolated ones, which is usually required for applications such as data storage, is still absent. Here, we show the controlled nucleation and motion of isolated three-fold vertices under an applied electric field. At the PbTiO 3 /SrRuO 3 interface, a two-unit-cell thick SrTiO 3 layer provides electrical boundary conditions for the formation of three-fold vertices. Utilizing the SrTiO 3 layer and in situ electrical testing system, we find that isolated three-fold vertices can move in a controllable and reversible manner with a velocity up to ~629 nm s -1 . Microstructural evolution of the nucleation and propagation of isolated three-fold vertices is further revealed by phase-field simulations. This work demonstrates the ability to electrically manipulate isolated three-fold vertices, shedding light on the dynamic property of isolated topological polar structures.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Tuning magnetoelectricity in a mixed-anisotropy antiferromagnet

Control of magnetization and electric polarization is attractive in relation to tailoring materials for data storage and devices such as sensors or antennae. In magnetoelectric materials, these degrees of freedom are closely coupled, allowing polarization to be controlled by a magnetic field, and magnetization by an electric field, but the magnitude of the effect remains a challenge in the case of single-phase magnetoelectrics for applications. We demonstrate that the magnetoelectric properties of the mixed-anisotropy antiferromagnet LiNi 1-x Fe x PO 4 are profoundly affected by partial substitution of Ni 2+ ions with Fe 2+ on the transition metal site. This introduces random site-dependent single-ion anisotropy energies and causes a lowering of the magnetic symmetry of the system. In turn, magnetoelectric couplings that are symmetry-forbidden in the parent compounds, LiNiPO 4 and LiFePO 4 , are unlocked and the dominant coupling is enhanced by almost two orders of magnitude. Our results demonstrate the potential of mixed-anisotropy magnets for tuning magnetoelectric properties.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Rapid sensing of hidden objects and defects using a single-pixel diffractive terahertz sensor

Abstract Terahertz waves offer advantages for nondestructive detection of hidden objects/defects in materials, as they can penetrate most optically-opaque materials. However, existing terahertz inspection systems face throughput and accuracy restrictions due to their limited imaging speed and resolution. Furthermore, machine-vision-based systems using large-pixel-count imaging encounter bottlenecks due to their data storage, transmission and processing requirements. Here, we report a diffractive sensor that rapidly detects hidden defects/objects within a 3D sample using a single-pixel terahertz detector, eliminating sample scanning or image formation/processing. Leveraging deep-learning-optimized diffractive layers, this diffractive sensor can all-optically probe the 3D structural information of samples by outputting a spectrum, directly indicating the presence/absence of hidden structures or defects. We experimentally validated this framework using a single-pixel terahertz time-domain spectroscopy set-up and 3D-printed diffractive layers, successfully detecting unknown hidden defects inside silicon samples. This technique is valuable for applications including security screening, biomedical sensing and industrial quality control.

Li, Jingxi (ORCID:0000000165958680)↗

Down-selection of biomolecules to assemble “reverse micelle” with perovskites

Abstract Biological molecule-semiconductor interfacing has triggered numerous opportunities in applied physics such as bio-assisted data storage and computation, brain-computer interface, and advanced distributed bio-sensing. The introduction of electronics into biological embodiment is being quickly developed as it has great potential in providing adaptivity and improving functionality. Reciprocally, introducing biomaterials into semiconductors to manifest bio-mimetic functionality is impactful in triggering new enhanced mechanisms. In this study, we utilize the vulnerable perovskite semiconductors as a platform to understand if certain types of biomolecules can regulate the lattice and endow a unique mechanism for stabilizing the metastable perovskite lattice. Three tiers of biomolecules have been systematically tested and the results reveal a fundamental mechanism for the formation of a “reverse-micelle” structure. Systematic exploration of a large set of biomolecules led to the discovery of guiding principle for down-selection of biomolecules which extends the classic emulsion theory to this hybrid systems. Results demonstrate that by introducing biomaterials into semiconductors, natural phenomena typically observed in biological systems can also be incorporated into semiconducting crystals, providing a new perspective to engineer existing synthetic materials.

59 BASIC BIOLOGICAL SCIENCES↗

Machine learning for automated experimentation in scanning transmission electron microscopy

Abstract Machine learning (ML) has become critical for post-acquisition data analysis in (scanning) transmission electron microscopy, (S)TEM, imaging and spectroscopy. An emerging trend is the transition to real-time analysis and closed-loop microscope operation. The effective use of ML in electron microscopy now requires the development of strategies for microscopy-centric experiment workflow design and optimization. Here, we discuss the associated challenges with the transition to active ML, including sequential data analysis and out-of-distribution drift effects, the requirements for edge operation, local and cloud data storage, and theory in the loop operations. Specifically, we discuss the relative contributions of human scientists and ML agents in the ideation, orchestration, and execution of experimental workflows, as well as the need to develop universal hyper languages that can apply across multiple platforms. These considerations will collectively inform the operationalization of ML in next-generation experimentation.

36 MATERIALS SCIENCE↗

Tunable quadruple-well ferroelectric van der Waals crystals

The family of layered thio- and seleno-phosphates has gained attention as potential control dielectrics for the rapidly growing family of two-dimensional and quasi-two-dimensional electronic materials. Here we report a combination of density functional theory calculations, quantum molecular dynamics simulations and variable-temperature, -pressure and -bias piezoresponse force microscopy data to predict and verify the existence of an unusual ferroelectric property—a uniaxial quadruple potential well for Cu displacements—enabled by the van der Waals gap in copper indium thiophosphate (CuInP 2 S 6 ). The calculated potential energy landscape for Cu displacements is strongly influenced by strain, accounting for the origin of the negative piezoelectric coefficient and rendering CuInP 2 S 6 a rare example of a uniaxial multi-well ferroelectric. Experimental data verify the coexistence of four polarization states and explore the temperature-, pressure- and bias-dependent piezoelectric and ferroelectric properties, which are supported by bias-dependent molecular dynamics simulations. As a result, these phenomena offer new opportunities for both fundamental studies and applications in data storage and electronics.

36 MATERIALS SCIENCE↗

Switchable geometric frustration in an artificial-spin-ice–superconductor heterosystem

Geometric frustration emerges when local interaction energies in an ordered lattice structure cannot be simultaneously minimized, resulting in a large number of degenerate states. The numerous degenerate configurations may lead to practical applications in microelectronics(1), such as data storage, memory and logic(2). However, it is difficult to achieve very high degeneracy, especially in a two-dimensional system(3,4). Here, we showcase in situ controllable geometric frustration with high degeneracy in a two-dimensional flux-quantum system. We create this in a superconducting thin film placed underneath a reconfigurable artificial-spin-ice structure(5). The tunable magnetic charges in the artificial-spin-ice strongly interact with the flux quanta in the superconductor, enabling switching between frustrated and crystallized flux quanta states. The different states have measurable effects on the superconducting critical current profile, which can be reconfigured by precise selection of the spin-ice magnetic state through the application of an external magnetic field. We demonstrate the applicability of these effects by realizing a reprogrammable flux quanta diode. The tailoring of the energy landscape of interacting 'particles' using artificial-spin-ices provides a new paradigm for the design of geometric frustration, which could illuminate a path to control new functionalities in other material systems, such as magnetic skyrmions(6), electrons and holes in two-dimensional materials(7,8), and topological insulators(9), as well as colloids in soft materials(10-13).

Wang, Yong-Lei (ORCID:0000000303917757)↗

Indefinite and bidirectional near-infrared nanocrystal photoswitching

Materials whose luminescence can be switched by optical stimulation drive technologies ranging from superresolution imaging, nanophotonics, and optical data storage, to targeted pharmacology, optogenetics, and chemical reactivity. Furthermore, these photoswitchable probes, including organic fluorophores and proteins, can be prone to photodegradation and often operate in the ultraviolet or visible spectral regions. Colloidal inorganic nanoparticles can offer improved stability, but the ability to switch emission bidirectionally, particularly with near-infrared (NIR) light, has not, to our knowledge, been reported in such systems. Here, we present two-way, NIR photoswitching of avalanching nanoparticles (ANPs), showing full optical control of upconverted emission using phototriggers in the NIR-I and NIR-II spectral regions useful for subsurface imaging. Employing single-step photodarkening and photobrightening, we demonstrate indefinite photoswitching of individual nanoparticles (more than 1,000 cycles over 7 h) in ambient or aqueous conditions without measurable photodegradation. Critical steps of the photoswitching mechanism are elucidated by modelling and by measuring the photon avalanche properties of single ANPs in both bright and dark states. Unlimited, reversible photoswitching of ANPs enables indefinitely rewritable two-dimensional and three-dimensional multilevel optical patterning of ANPs, as well as optical nanoscopy with sub-Å localization superresolution that allows us to distinguish individual ANPs within tightly packed clusters.

36 MATERIALS SCIENCE↗

Electrically driven deep ultraviolet MgZnO lasers at room temperature

Semiconductor lasers in the deep ultraviolet (UV) range have numerous potential applications ranging from water purification and medical diagnosis to high-density data storage and flexible displays. Nevertheless, very little success was achieved in the realization of electrically driven deep UV semiconductor lasers to date. Here, we report the fabrication and characterization of deep UV MgZnO semiconductor lasers. These lasers are operated with continuous current mode at room temperature and the shortest wavelength reaches 284 nm. The wide bandgap MgZnO thin films with various Mg mole fractions were grown on c-sapphire substrate using radio-frequency plasma assisted molecular beam epitaxy. Metal-semiconductor-metal (MSM) random laser devices were fabricated using lithography and metallization processes. Besides the demonstration of scalable emission wavelength, very low threshold current densities of 29-33 A/cm 2 are achieved. Furthermore, numerical modeling reveals that impact ionization process is responsible for the generation of hole carriers in the MgZnO MSM devices. The interaction of electrons and holes leads to radiative excitonic recombination and subsequent coherent random lasing.

36 MATERIALS SCIENCE↗

Accurate and confident prediction of electron beam longitudinal properties using spectral virtual diagnostics

Abstract Longitudinal phase space (LPS) provides a critical information about electron beam dynamics for various scientific applications. For example, it can give insight into the high-brightness X-ray radiation from a free electron laser. Existing diagnostics are invasive, and often times cannot operate at the required resolution. In this work we present a machine learning-based Virtual Diagnostic (VD) tool to accurately predict the LPS for every shot using spectral information collected non-destructively from the radiation of relativistic electron beam. We demonstrate the tool’s accuracy for three different case studies with experimental or simulated data. For each case, we introduce a method to increase the confidence in the VD tool. We anticipate that spectral VD would improve the setup and understanding of experimental configurations at DOE’s user facilities as well as data sorting and analysis. The spectral VD can provide confident knowledge of the longitudinal bunch properties at the next generation of high-repetition rate linear accelerators while reducing the load on data storage, readout and streaming requirements.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Surface localized magnetism in transition metal doped alumina

Alumina is a structural ceramic that finds many uses in a broad range of applications. It is widely employed in the aerospace and biomedical sectors due to its stability at high temperatures and in harsh chemical environments. Here, we show that magnetism can be induced at alumina surfaces by doping with 3d transition metals. We analyze the electronic structure, spin magnetic moments, and spin density of α-Al 2 O 3 as a function of both dopant species (Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu) and depth using first principles calculations. Our results show that all dopants, with the exception of Sc, produce magnetic moments that are concentrated to the surface of alumina with varying degrees of delocalization. It is seen that all of the dopants are at least meta-stable on the surface and must overcome an energy barrier of 0.19–1.14 eV in order to diffuse from the surface into the bulk. As a result of judiciously doping with select 3$\textit{d}$ transition metals the surface of alumina can be made magnetic. This could lead to novel applications in data storage, catalysis, and biomedical engineering through an added surface functionality.

36 MATERIALS SCIENCE↗

Probing ferroelectric domain structures and their switching dynamics in SrBi2Ta2O9 by in-situ electric biasing in transmission electron microscopy

Abstract Lead-free SrBi 2 Ta 2 O 9 (SBT) has been a promising ferroelectric material for various applications such as electronics and data storage due to its outstanding ferroelectric properties including high fatigue endurance and low leakage current. However, the atomic-scale domain structure and switching dynamics of ferroelectric SBT remain elusive. This study reveals that spontaneous polarization arises from canted bismuth-cation displacements, forming 90° and Ising-type 180° domain walls. Interestingly, topological pairs of ferroelectric vortex and antivortex connect ferroelectric boundaries where three domain walls converge. In situ electrical biasing transmission electron microscopy (TEM) reveals the dominance of 180° switching over 90°, where oxygen octahedral connectivity is protected by ferroelastic energy in the 90° domain wall. Consequently, all 180° domain walls and (anti)vortices are removed, leaving only 90° domain walls in the electrically poled states. Chemical deterioration along domain walls highlights vulnerability of SBT to ferroelectric fatigue. This study provides insight into crucial aspects for practical applications of SBT.

36 MATERIALS SCIENCE↗

Polarization selective phase-change nanomodulator

Manipulating optical signals below the diffraction limit is crucial for next-generation data-storage and telecommunication technologies. Although controlling the flow of light around nanoscale waveguides was achieved over a decade ago, modulating optical signals at terahertz frequencies within nanoscale volumes remains a challenge. Since the physics underlying any modulator relies on changes in dielectric properties, the incorporation of strongly electron-correlated materials (SECMs) has been proposed because they can exhibit orders of magnitude changes in electrical and optical properties with modest thermal, electrical or optical trigger signals. Here we demonstrate a hybrid nanomodulator of deep sub-wavelength dimensions with an active volume of only 0.002 µm 3 by spatially confining light on the nanometre length scale using a plasmonic nanostructure while simultaneously controlling the reactive near-field environment at its optical focus with a single, precisely positioned SECM nanostructure. Since the nanomodulator functionality hinges on this near-field electromagnetic interaction, the modulation is also selectively responsive to polarization. Lastly, this architecture suggests one path for designing reconfigurable optoelectronic building blocks with responses that can be tailored with exquisite precision by varying size, geometry, and the intrinsic materials properties of the hybrid elements.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Synthetic magnetoelectric coupling in a nanocomposite multiferroic

Given the paucity of single phase multiferroic materials (with large ferromagnetic moment), composite systems seem an attractive solution to realize magnetoelectric coupling between ferromagnetic and ferroelectric order parameters. Despite having antiferromagnetic order, BiFeO₃ (BFO) has nevertheless been a key material due to excellent ferroelectric properties at room temperature. We studied a superlattice composed of 8 repetitions of 6 unit cells of La₀.₇Sr₀.₃MnO₃ (LSMO) grown on 5 unit cells of BFO. Significant net uncompensated magnetization in BFO, an insulating superlattice, is demonstrated using polarized neutron reflectometry. Remarkably, the magnetization enables magnetic field to change the dielectric properties of the superlattice, which we cite as an example of synthetic magnetoelectric coupling. Importantly, controlled creation of magnetic moment in BFO is a much needed path toward design and implementation of integrated oxide devices for next generation magnetoelectric data storage platforms.

36 MATERIALS SCIENCE↗