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At least 109 records · Page 6

Optical-Frequency Magnetic Polarizability in a Layered Semiconductor

The optical response of crystals is most commonly attributed to electric dipole interactions between light and matter. Although metamaterials support “artificial” magnetic resonances supported by mesoscale structuring, there are no naturally occurring materials known to exhibit a nonzero optical-frequency magnetic polarizability. Here, we experimentally demonstrate and quantify a naturally occurring nonzero magnetic polarizability in a layered semiconductor system: two-dimensional (Ruddlesden-Popper phase) hybrid organic-inorganic perovskites. These results demonstrate the only known material with an optical-frequency permeability that differs appreciably from vacuum, informing future efforts to find, synthesize, or exploit atomic-scale optical magnetism for novel optical phenomena such as negative index of refraction and electromagnetic cloaking.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Design of space-type electronic power transformers

Both open and encapsulated varieties of high reliability, low weight, and high efficiency moderate and high voltage transformers were investigated to determine the advantages and limitations of their construction in the ranges of power and voltage required for operation in the hard vacuum environment of space. Topics covered include: (1) selection of the core material; (2) preliminary calculation of core dimensions; (3) selection of insulating materials including magnet wire insulation, coil forms, and layer and interwinding insulation; (4) coil design; (5) calculation of copper losses, core losses and efficiency; (6) calculation of temperature rise; and (7) optimization of design with changes in core selection or coil design as required to meet specifications.

Ahearn, J. F.↗

Epitaxial 2D Magnet and Topological Insulator Heterostructures

I will discuss our latest advances on the epitaxial growth of 2D van der Waals (vdW) magnets and their integration with topological insulators (TI). This work is motivated by the realization of topological phases such as the quantum anomalous Hall effect and highly efficient spin-orbit torque produced by TIs. Our initial studies of MnSe2 growth on Bi2Se3 showed a tendency for the interdiffusion of Mn into the Bi2Se3. This ultimately led to the synthesis of MnBi2Se4 (MBS), a new magnetic TI. Interestingly, the vdW phase is not the thermodynamically stable phase and bulk crystals do not exist, so the epitaxial stabilization of MBS creates the opportunity to explore the magnetic and topological properties of this material. We find that MBS is a layered antiferromagnet, similar to MnBi2Te4, but a difference is that the magnetic moments lie in the plane of the film. Angle resolved photoemission experiments show the presence of a topological surface state with Dirac dispersion. For bilayers of 2D magnets and TIs, we have developed FGT films on Bi2Te3. We first optimized FGT by studying its growth on Ge(111) substrates, where we find that kinetic considerations play a major role. Using cross-sectional scanning transmission electron microscopy and scanning tunneling microscopy, we optimize the FGT films to have atomically smooth surfaces and abrupt interfaces with the Ge(111). Subsequently, we have developed the growth of FGT on Bi2Te3 for the integration of 2D magnets with Tis. Interestingly, we observe room temperature ferromagnetism in FGT/Bi2Te3 heterostructures by varying the growth conditions.

Kawakami, Roland↗

Low-dimensional metal–organic frameworks: a pathway to design, explore and tune magnetic structures

Here, the magnetic structure adopted by a material relies on symmetry, the hierarchy of exchange interactions between magnetic ions and local anisotropy. A direct pathway to control the magnetic interactions is to enforce dimensionality within the material, from zero-dimensional isolated magnetic ions, one-dimensional (1D) spin-chains, two-dimensional (2D) layers to three-dimensional (3D) order. Being able to design a material with a specific dimensionality for the phenomena of interest is non-trivial. While many advances have been made in the area of inorganic magnetic materials, organic compounds offer distinct and potentially more fertile ground for material design. In particular magnetic metal–organic frameworks (mMOFs) combine magnetism with non-magnetic property functionality on the organic linkers within the structural framework, which can further be tuned with mild perturbations of pressure and field to induce phase transitions. Here, it is examined how neutron scattering measurements on mMOFs can be used to directly determine the magnetic structure when the magnetic ions are in a 2D layered environment within the wider 3D crystalline framework. The hydrated formate, in deuterated form, Co(DCOO) 2 ·2D 2 O, which was one of the first magnetic MOFs to be investigated with neutron diffraction, is reinvestigated as an exemplar case.

magnetism↗

Magnetic excitations in infinite-layer nickelates

The discovery of superconductivity in infinite-layer nickelates brings us tantalizingly close to a material class that mirrors the cuprate superconductors. We measured the magnetic excitations in these nickelates using resonant inelastic x-ray scattering at the Ni L 3 -edge. Undoped NdNiO 2 possesses a branch of dispersive excitations with a bandwidth of approximately 200 milli–electron volts, which is reminiscent of the spin wave of strongly coupled, antiferromagnetically aligned spins on a square lattice. The substantial damping of these modes indicates the importance of coupling to rare-earth itinerant electrons. Upon doping, the spectral weight and energy decrease slightly, whereas the modes become overdamped. Our results highlight the role of Mottness in infinite-layer nickelates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Layer Hall effect in a 2D topological axion antiferromagnet

While ferromagnets have been known and exploited for millennia, antiferromagnets (AFMs) were only discovered in the 1930s. The elusive nature indicates AFMs' unique properties: At large scale, due to the absence of global magnetization, AFMs may appear to behave like any non-magnetic material; However, such a seemingly mundane macroscopic magnetic property is highly nontrivial at microscopic level, where opposite spin alignment within the AFM unit cell forms a rich internal structure. In topological AFMs, such an internal structure leads to a new possibility, where topology and Berry phase can acquire distinct spatial textures. Here, we study this exciting possibility in an AFM Axion insulator, even-layered MnBi 2 Te 4 flakes, where spatial degrees of freedom correspond to different layers. Remarkably, we report the observation of a new type of Hall effect, the layer Hall effect, where electrons from the top and bottom layers spontaneously deflect in opposite directions. Specifically, under no net electric field, even-layered MnBi 2 Te 4 shows no anomalous Hall effect (AHE); However, applying an electric field isolates the response from one layer and leads to the surprising emergence of a large layer-polarized AHE (~50e 2 /h). Such a layer Hall effect uncovers a highly rare layer-locked Berry curvature, which serves as a unique character of the space-time PT-symmetric AFM topological insulator state. Moreover, we found that the layer-locked Berry curvature can be manipulated by the Axion field, E∙B, which drives the system between the opposite AFM states. Our results achieve previously unavailable pathways to detect and manipulate the rich internal spatial structure of fully-compensated topological AFMs. The layer-locked Berry curvature represents a first step towards spatial engineering of Berry phase, such as through layer-specific moiré potential.

36 MATERIALS SCIENCE↗

Super-moiré spin textures in twisted two-dimensional antiferromagnets

Stacking two-dimensional layered materials offers a platform to engineer electronic and magnetic states. In general, the resulting states—such as moiré magnetism—have a periodicity at the length scale of the moiré unit cell. Here we study magnetic order in twisted double-bilayer chromium triiodide by means of scanning nitrogen-vacancy microscopy. We observe long-range magnetic textures extending beyond the single moiré unit cell, which we dub a super-moiré magnetic state. At small twist angles, the size of the spontaneous magnetic texture increases with twist angle, opposite to the underlying moiré wavelength. The spin-texture size reaches a maximum of about 300 nm in 1.1° twisted devices, an order of magnitude larger than the underlying moiré wavelength, and vanishes at twist angles above 2°. The obtained magnetic field maps suggest the formation of antiferromagnetic Néel-type skyrmions spanning multiple moiré cells. The twist-angle-dependent study, combined with large-scale atomistic Monte Carlo simulations, suggests that the magnetic competition between the Dzyaloshinskii–Moriya interaction, magnetic anisotropy and exchange interactions—which all depend on the relative rotation of the layers—produces the topological textures that emerge in the super-moiré spin order.

Wong, King Cho [Univ. of Stuttgart (Germany)] (ORC↗

Colossal Magnetoresistance without Mixed Valence in a Layered Phosphide Crystal

Materials with strong magnetoresistive responses are the backbone of spintronic technology, magnetic sensors, and hard drives. Among them, manganese oxides with a mixed valence and a cubic perovskite structure stand out due to their colossal magnetoresistance (CMR). A double exchange interaction underlies the CMR in manganates, whereby charge transport is enhanced when the spins on neighboring Mn 3+ and Mn 4+ ions are parallel. Prior efforts to find different materials or mechanisms for CMR resulted in a much smaller effect. Here an enormous CMR at low temperatures in EuCd 2 P 2 without manganese, oxygen, mixed valence, or cubic perovskite structure is shown. EuCd 2 P 2 has a layered trigonal lattice and exhibits antiferromagnetic ordering at 11 K. The magnitude of CMR (10(4)%) in as-grown crystals of EuCd 2 P 2 rivals the magnitude in optimized thin films of manganates. In this work, the magnetization, transport, and synchrotron X-ray data suggest that strong magnetic fluctuations are responsible for this phenomenon. The realization of CMR at low temperatures without heterovalency leads to a new regime for materials and technologies related to antiferromagnetic spintronics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Phonon dynamics in quantum spin liquid and valence bond crystal states in the barlowite family of kagome magnets

The barlowite [Cu 4 ⁢(OD) 6⁢ FBr] family of materials is characterized by antiferromagnetic spin-1/2 kagome layers and are believed to host interesting ground states of quantum magnetism. Substituting the interlayer sites with zinc ions yields Zn-barlowite (Zn 𝑥 ⁢Cu 4−𝑥 ⁢(OD) 6 ⁢FBr, 𝑥 ≈ 0.80) which is a strong candidate to have a quantum spin liquid (QSL) state. Experimentally distinguishing between valence bond crystal (VBC) and QSL states in the absence of magnetic ordering can prove challenging as both states exhibit similar average spin-spin correlations. Using high-resolution inelastic x-ray scattering with 1.4 meV energy resolution, we probe acoustic phonons in these structurally similar materials at various temperatures. Our measurements uncover robust differences possibly driven by different spin-phonon physics in VBC and QSL states, particularly at the 𝑀-point Brillouin zone boundary. Over a large 𝑇=[15,200]⁢ K temperature range, where neither material undergoes magnetic ordering nor a structural transition, we observe phonon softening in Zn-barlowite in contrast to a hardening of the same phonon in barlowite. Further, these results indicate that acoustic phonons in the barlowite system can be used to study and possibly distinguish between QSL and disordered VBC states in quantum magnets.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Identifying Strain Stacking Boundaries between Multiphase Domains in Atomically Thin Two-Dimensional Magnets

Stacking engineering of van der Waals materials is an important strategy to control the materials’ properties, such as electronic correlations, ferroelectricity, and layer-dependent two-dimensional magnetism. A timely testbed for the study of the latter is atomically thin chromium trihalides (CrX 3 , X = Cl, Br, I). Notably, by understanding the sliding mechanism between different stacking sequences, control of the stacking arrangement, and thus magnetic properties in CrX 3 , can be achieved. Such insight, however, is currently lacking. Here, in this study, advanced electron microscopy methods are used to identify multiple stacking sequences corresponding to different bulk phases in atomically thin CrX 3 (X = Cl and Br) down to bilayer thickness and with lateral domain sizes as small as tens of nanometers. Indications of nanometer scale transitions and interactions at the stacking boundaries are found, including a universally preferred sliding direction that is consistent with density functional theory calculations and the strain fields at lateral heterostructure boundaries. This study demonstrates the necessity to consider local stacking structures when interpreting averaged magnetic properties measured with macroscale probes. Additionally, the preferred sliding direction insight from this study provides a strategy to control stacking sequence in atomically thin CrX 3 samples during the exfoliation and sample fabrication process.

DFT calculations↗

The role of microstructural evolution during spark plasma sintering on the soft magnetic and electronic properties of a CoFe–Al2O3 soft magnetic composite

Abstract For transformers and inductors to meet the world’s growing demand for electrical power, more efficient soft magnetic materials with high saturation magnetic polarization and high electrical resistivity are needed. This work aimed at the development of a soft magnetic composite synthesized via spark plasma sintering with both high saturation magnetic polarization and high electrical resistivity for efficient soft magnetic cores. CoFe powder particles coated with an insulating layer of Al 2 O 3 were used as feedstock material to improve the electrical resistivity while retaining high saturation magnetic polarization. By maintaining a continuous non-magnetic Al 2 O 3 phase throughout the material, both a high saturation magnetic polarization, above 1.5 T, and high electrical resistivity, above 100 μΩ·m, were achieved. Through microstructural characterization of samples consolidated at various temperatures, the role of microstructural evolution on the magnetic and electronic properties of the composite was elucidated. Upon consolidation at relatively high temperature, the CoFe was to found plastically deform and flow into the Al 2 O 3 phase at the particle boundaries and this phenomenon was attributed to low resistivity in the composite. In contrast, at lower consolidation temperatures, perforation of the Al 2 O 3 phase was not observed and a high electrical resistivity was achieved, while maintaining a high magnetic polarization, ideal for more efficient soft magnetic materials for transformers and inductors.

36 MATERIALS SCIENCE↗

Dynamic signatures of spin-lattice coupling in the layered ferrimagnet Mn 3 Si 2 Te 6

Magnetic van der Waals (vdW) materials exhibit a profound interconnectedness between their various degrees of freedom, pointing to a wealth of potential applications in low-power and high-speed spintronic devices. Recently, light-matter interactions have been leveraged as robust, dynamic pathways to gain control over the properties of vdW magnets through the use of ultrafast pulses of light. Here, we utilize ultrafast photoexcitation to drive coherent lattice oscillations in the layered ferrimagnetic crystal Mn 3 Si 2 Te 6 , which significantly stiffen below the magnetic ordering temperature. We suggest that this is due to an exchange-mediated contraction of the lattice, stemming from strong magneto-structural coupling in this material. Furthermore, simulations of the transient incoherent response uncover the critical role of the spin-mediated electronic relaxation pathways. These results underscore the importance of spin-lattice coupling in vdW magnets and demonstrate a promising strategy for their dynamic optical control via their entangled degrees of freedom.

36 MATERIALS SCIENCE↗

Variation of Aliphatic Diisocyanates in Bio-Based TPUs

The utilization of bio-based materials for polymer production poses a challenge to both the industrial and academic sectors due to the availability and production costs of the necessary raw materials. Diisocyanates necessary for polyurethane synthesis have posed a particular challenge, given the paucity of natural diamine precursors for traditional phosgenation. We recently developed a phosgene-free flow chemistry methodology that allows for the safe, efficient, and scalable preparation of diisocyanates from naturally produced diacids. This chemistry broadens the potential for the development of renewable diisocyanates for a broad variety of applications. Here, we expand upon this work by demonstrating the scaled production of a panel of bio-based linear, aliphatic diisocyanates, with chain lengths ranging from four to eight carbons in good yields of 57–81% and high purity (~97%). Furthermore, these are applied to the synthesis of thermoplastic polyurethanes (TPUs) containing up to a 100% renewable carbon content. TPUs formulated using shorter carbon-chained diisocyanates displayed a higher tensile strength compared to those formulated using longer chains. Ready access to diisocyanates of varying chain length affords the ability to tailor TPU properties through careful selection of the diisocyanate, polyol, and chain extender, offering hard and soft TPUs for multiple end-use applications.

36 MATERIALS SCIENCE↗

Self-Powered Autonomous Sensing System for Arctic Ocean using a Frequency-multiplied Cylindrical Triboelectric Nanogenerator

An autonomous sensing system for collecting environmental observations in the Arctic region is critical for the estimation and prediction of climate change. Ocean waves are a great source of energy for these sensing systems but there has been limited research done on small-scale energy harvesting applications in the Arctic Ocean (subsea or surface). The available wave energy in the Arctic Ocean is lower than the typical ocean wave energy due to the low wave frequency, height, and operating months. Although the available wave energy depends on the specific location in the Arctic Ocean, the wave height decreases everywhere during the winter (Jan-March) [1]. Our target location in this work is the Beaufort and Chukchi Seas, which are ice covered for about 195 days per year leaving only a few months (June-November) for wave energy harvesting [2]. During these few months, the average wave frequency is 0.2 Hz and the most common wave frequency is around 0.15 Hz. Many energy harvesting methods are unsuitable for use in the Arctic Ocean because of to the cold temperature, low wave frequency, and low wave height. Triboelectric nanogenerators (TENG) are one of the few energy harvesting methods that excel in these conditions. Zhong et al. [3] designed a stacked pendulum-structured TENG for low-frequency ocean wave energy and reported the device generated a peak power density of 11.2 W/m3 under the low wave frequency of 0.2 Hz. The autonomous sensing system we developed for the Arctic Ocean, the Arctic-TENG, is based on a frequency-multiplied cylindrical TENG (FMC-TENG) which is an optimized TENG configuration for Arctic Ocean conditions due to the high power density under low-frequency wave conditions [4]. Figure 1 shows an FMC-TENG with multiple pairs of free-standing triboelectric-layer mode materials (Aluminum and FEP). The mass and magnet attached to the rotor store gravitational potential energy which is released as kinetic energy when the potential energy overcomes the repulsive magnetic force generated by the opposing magnet attached to the stator. This force unbalance triggers a sudden rotation and swinging motion of the mass which increases the angular velocity of the system and therefore enhances the output power of the TENG system. The main components of the Arctic-TENG are a 3D-printed rotor and stator, electric and dielectric material adhesive tape, and bearings. All these materials were cold-soaked and tested at -40 °C in a chest freezer. Both the 3D-printed parts and adhesives were confirmed to have a minimal effect from the cold temperature. Multiple bearings were tested and the starting torque of each one was compared both at room temperature and -40 °C. The bearing with the lowest starting torque at -40 °C was selected for use in the Arctic-TENG. The Arctic-TENG was tested using an out-of-water motor-driven wave simulator (Figure 2). The wave simulator allows for controlled testing at a wave height of 0.2 m and frequencies between 0.1 Hz to 0.5 Hz. This wave simulator was used for both room temperature and -40 °C testing. The Arctic-TENG generated significantly more power at -40 °C compared to room temperature for each frequency tested. The system stored energy in a supercapacitor via a power management circuit, and the amount of energy stored per day was calculated at different wave frequencies. Based on the conditions at the proposed deployment location (days of non-ice-covered ocean and wave frequency), the amount of stored energy per year from Arctic-TENG was calculated to be enough energy for two transmissions every day. Durability testing was completed on the Arctic-TENG at room temperature to determine the lifetime. The rotor of the Arctic-TENG was attached to a DC motor and spun continuously for several millions of cycles without degradation of the electrical output, demonstrating the feasibility for long-term operation.

Jung, Hyunjun↗

Visualizing the Effect of Oxidation on Magnetic Domain Behavior of Nanoscale Fe 3 GeTe 2 for Applications in Spintronics

Magnetic van der Waals (vdW) materials offer an opportunity to design heterostructures that will lead to exotic functionalities that arise from interfacial interaction. In addition to coupling to different vdW materials, the naturally oxidized surface layer of a vdW material also forms a heterostructure with its bulk film, giving rise to intriguing phenomena. Here, we directly observe the impact of oxidation on the magnetic domains, namely, magnetic stripe domain and skyrmions, in a nanoscale Fe 3 GeTe 2 flake using cryo Lorentz transmission electron microscopy. After the Fe 3 GeTe 2 is exposed to ambient conditions, partial oxidation leads to an increase in the density of skyrmions even under zero magnetic field. Complete oxidation leads to a loss of the magnetic domain structure. We observe a gradual change in Fe 3 GeTe 2 from single crystal to amorphous as the oxidation increases. The oxidized Fe 3 GeTe 2 primarily consists of iron oxide, which could be antiferromagnetic in nature. We hypothesize that the interfacial interaction between these surface antiferromagnetic oxides and the bulk ferromagnetic Fe 3 GeTe 2 , as well as the effect of interfacial roughness, leads to the increase in Néel skyrmion creation. Furthermore, this work opens a path to harness controlled oxidation as a build block to create dense skyrmion lattices without the need for an external magnetic field, leading to potential future applications in spintronic devices.

36 MATERIALS SCIENCE↗

Multi-scale nonlinear stress analysis of Nb 3 Sn superconducting accelerator magnets

A multi-scale nonlinear procedure to analyze the stress in Nb 3 Sn superconducting accelerator magnets is presented to address one of the most challenging obstacles currently facing the successful development of high-field superconducting magnets—the issue of stress management. The study demonstrates that gaskets (special nonlinear materials) are capable of modeling the complex nonlinear deformation behavior of insulation layers within the Nb 3 Sn coil block and that Hill materials (orthotropic materials utilizing the Hill yield criterion) are suitable to enable homogenization of the filamentary regions and the resin-impregnated Nb 3 Sn Rutherford cables. With the whole magnet under preload, cool-down, and Lorentz forces, the nonlinear behavior of the Nb 3 Sn coil was simulated, in three orthongonal axes, by the combined properties of the gaskets (insulation layers) and Hill materials (resin-impreganted cable). The procedure entailes minimal material assumptions because it incorporated measured stress-strain curves in the analysis. The coil was simulated to a high level of detail consisting of the insulation layers and resin-impregnated cables. The computed compressive azimuthal stresses of the cables were used to assess the stress-induced performance degradation. Through submodeling, the area-weighted average axial strains of the strands were computed and employed to evaluate the strain-induced performance degradation. The overall performance degradation of the Nb 3 Sn coil was thus obtained, and this information was subsequently used to guide the design of the overall magnet. Besides Nb 3 Sn magnets, this procedure can also be employed in the design of LTS, HTS, and room temperature magnets or in any composite structures.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

The transient properties of 2D magnets: from mechanical exfoliation to ultrafast optical spectroscopy of CrX 3 materials

The discovery of two-dimensional (2D) systems hosting intrinsic long-range magnetic order represents a seminal achievement, adding to the already diverse array of physics supported by layered van der Waals (vdW) materials. This finding has spurred great interest among the research community, with efforts aimed at uncovering their fundamental properties and light- matter interactions. A prototypical example of a 2D magnetic material is Crl 3 , where the strong relationship between crystalline structure and magnetic order, along with strong light- matter interactions, provide a promising platform to explore the nature of couplings between magnetism and the other degrees of freedom at the 2D limit. In this report, we highlight our efforts involving the use of time-resolved magneto-optical Kerr effect (TR-MOKE) spectroscopy to probe the magnetization and vibrational dynamics of Crl 3 . These measurements reveal evidence of strong exchange-mediated coupling between lattice vibrations and spin oscillations. Additionally, we discuss our related efforts to explore other material from the Chromium trihalide family through mechanical exfoliation to support subsequent optical spectroscopy investigations.

36 MATERIALS SCIENCE↗