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At least 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Stacking Faults and Short-Range Magnetic Correlations in Single Crystal Y 5 Ru 2 O 12 : A Structure with Ru +4.5 One-Dimensional Chains

In this paper, the synthesis, structure, and physical properties of Y 5 Ru 2 O 12 , a new member of the Ln 5 B 2 O 12 class (Ln = lanthanide, B = Ru, Re, Mo) are reported. Single crystals of Y 5 Ru 2 O 12 are synthesized using a high-temperature, high-pressure (700 °C, 200 MPa) hydrothermal method. The structure features edge-sharing Ru—O—Ru 1D chains of distorted RuO6 octahedra. The YO n (n = 6 and 7) polyhedral groups bridge Ru—O—Ru chains across the unit cell by forming a complex 3D structure. The Ru—O—Ru chains contain alternating shorter and longer Ru—Ru distances along the chain. Single crystal neutron diffraction shows streak-like diffuse scattering along the H-direction, due to stacking faults. Temperature-dependent anisotropic magnetic measurements reveal a broad feature over a wide temperature range, with a maximum at ≈70 K indicating potential short-range ordering, with canted antiferromagnetic behavior below 30 K. The dominant magnetic interactions are antiferromagnetic with a large negative Weiss temperature θ ≈ –200 K. The compound has an effective magnetic moment that is anomalously large for this class of compounds (≈4 μ B Ru –1 ), and a phenomenological spin Hamiltonian describing the unusual anisotropic magnetization of Y 5 Ru 2 O 12 is proposed.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Magnetic transitions and magnetocaloric effect of Gd 4 Nd 1 Si 2 Ge 2

In this work, crystal structure and magnetic properties of the quaternary Gd 4 Nd 1 Si 2 Ge 2 compound were investigated using synchrotron X-ray diffraction and magnetic measurements. The compound crystallized into an orthorhombic structure in the temperature range 200-300 K. In zero field cooling, the compound undergoes a spin reorientation following a ferromagnetic-like transition at 276 K. The spin reorientation is hinted at by nonlinear changes of lattice parameters but is suppressed in a high magnetic field of 6 T. Magnetic measurements revealed a magnetocaloric effect with a high relative cooling power. It is suggested that Nd substitution for Gd enlarges magnetic anisotropy and induces a canted spin structure.

36 MATERIALS SCIENCE↗
DOE OSTI2020

63,65 Cu NMR study of the magnetically ordered state of the multiferroic CuFeO 2

In this work, field-swept 63,65 Cu NMR spectra under magnetic fields up to 8.3 T at a constant NMR frequency and temperatures T < 12 K on a single crystalline sample of multiferroic CuFeO 2 were measured and analyzed. When the magnetic field is applied along the c axis, a nearly zero internal magnetic field at the Cu site in magnetic ordered state was observed. This is explained by the perfect cancellation of the internal fields produced by the 6 nearest neighbor Fe 3+ ( S = 5/2) ions, revealing the magnetic structure to be a collinear four-sublattice structure. On the other hand, when the magnetic field is applied along the ab plane, we observed a finite internal field at the Cu sites, which is due to the canting of the Fe moments. Strong change in the NMR signal intensity is observed around 7–8 T, corresponding to the magnetic phase transition from the collinear magnetic to ferroelectric incommensurate states. The ratio of the two magnetic phases significantly depends on the history of the change in the external magnetic field and the temperature of the sample. The details of history dependence of the ratio were discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2020

A non-intrusive optical (NIO) approach to characterize heliostats in utility-scale power tower plants: Sensitivity study

Power towers, a type of concentrating power tower technology, use a large number of heliostats to concentrate sunlight and produce renewable energy. Optical errors of heliostats can cause drastic losses in the efficiency of power-tower plants. Accurately measuring optical errors is crucial to assessing and improving plant performance. This analysis discusses an innovate non-intrusive optical (NIO) approach to measure slope, canting, and tracking errors by detecting distortions in the reflected tower structure in heliostat images. Further in this work a sensitivity study is carefully conducted to determine the uncertainty requirements to allow the method to calculate slope errors with an accuracy of 0.25 mrad. Measurement uncertainty sources include camera resolution and position uncertainty, tower position uncertainty, and number of collected images. Each uncertainty source is investigated to determine its impact on the accuracy of the slope-error calculation. A combination of theoretical results and experimental results obtained from data collected on a heliostat at Sandia National Laboratories is used to determine and validate uncertainty requirements. The analysis shows that a measurement uncertainty of 0.25 mrad can be realized by realistically controlling uncertainty sources when implementing the NIO method. It demonstrates the superior performance of NIO in performing in-situ optical characterization.

14 SOLAR ENERGY↗
DOE OSTI2021

A non-intrusive optical approach to characterize heliostats in utility-scale power tower plants: Flight path generation/optimization of unmanned aerial systems

A newly developed in situ non-intrusive optical (NIO) approach has been developed to survey various types of heliostat optical errors for a concentrating solar power (CSP) tower plant. To measure mirror surface slope error, facet canting error, and heliostat tracking error at a sub-milliradian accuracy, NIO requires several reflection images scanned over each individual heliostat. For a utility-scale plant that typically includes more than 10,000 heliostats, an unmanned aerial system (UAS) is crucial for efficient implementation of the NIO method. Here, we develop a flight path generation/optimization algorithm to plan more efficient UAS paths to collect NIO data over a utility-scale heliostat field. The algorithm considers NIO data requirements, all potential constraints, optimization within each subfield, and operational flexibility. Case studies are presented to illustrate the feasibility and robustness of the developed flight path algorithm. The path planning algorithm may also find applications elsewhere, such as drone-driven imaging under extreme conditions.

14 SOLAR ENERGY↗
DOE OSTI2022

Eu 5 Al 3 Sb 6 : Al 4 Tetrahedra Embedded in a Rock-Salt-Like Structure

The new Eu 5 Al 3 Sb 6 phase has been successfully synthesized as a pure phase through Sn flux methods yielding large, high-quality crystals. This structure type features disordered Al clusters that appear in the form of dual tetrahedra. It crystallizes in the monoclinic C2/m space group exhibiting a rock-salt-like Eu–Sb framework with [Al 4 ] tetrahedra replacing some of the cationic Eu atoms (space group: C2/m, a = 8.151(1) Å, b = 14.181(2) Å, c = 8.145(1) Å, β = 109.577(2)°). The structure models the [Al 4 ] as dual tetrahedra with the Al atom sites 37.5% occupied along with Eu present on the central site at 8% occupancy and the remainder of the site being vacant. The presence of the [Al 4 ] cluster is further supported by HRTEM. Electronic structure calculations show that this material is a semimetal with observed band crossings close to the Fermi level. Strong Al–Sb antibonding interactions were found from COHP calculations close to the Fermi level and provide the rationale for the deficiency of the Al cluster. Mössbauer spectroscopy on Eu-151 and Sb-121 provides oxidation states of 2+ and 3– along with the local environment. Magnetic susceptibility measurements can be described well with a Curie–Weiss law where an effective moment of 7.80 μB/mol Eu is obtained, consistent with Eu 2+ , and show canted antiferromagnetic behavior below 10 K. Temperature dependent resistivity shows a Kondo-like low-temperature upturn caused by enhanced scattering of the itinerant electrons with the 4f orbitals of Eu.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Exploring the Links between Structural Distortions, Orbital Ordering, and Multipolar Magnetic Ordering in Double Perovskites Containing Re(VI) and Os(VII)

A combination of high-resolution powder diffraction techniques and solid-state NMR has been employed to explore the links between crystal structure, orbital ordering, and magnetism in three isostructural double perovskites containing transition metal ions with a 5d 1 configuration. In Ba 2 ZnReO 6 , both neutron and synchrotron X-ray powder diffraction data reveal a cubic-to-tetragonal transition at 23 K that breaks the degeneracy of the t 2g orbitals and leads to a pattern of orbital ordering that stabilizes magnetic ordering when the sample is cooled below 16 K. Similar behavior is observed in Ba 2 MgReO 6 , with an orbital ordering temperature of 33 K and a magnetic ordering temperature of 18 K. Prior theoretical works suggest that the pattern of orbital order seen in the P42/mnm space group is needed to stabilize the heavily canted antiferromagnetism of these compounds. Unfortunately, powder diffraction data is not sensitive enough to differentiate between the I4/mmm and P42/mnm structural models, as the distortions are too subtle to be unambiguously identified from either neutron or synchrotron X-ray powder diffraction methods. In contrast, both diffraction and 7 Li NMR data indicate that Ba 2 LiOsO 6 retains the cubic structure down to 1.7 K. The antiferromagnetic ground state and lack of any sign of orbital ordering in Ba 2 LiOsO 6 provide compelling evidence that the electronically driven tetragonal distortion seen in Ba2ZnReO6, and Ba2MgReO6 is intimately linked to the magnetic ordering seen in those compounds. The absence of magnetic reflections in high intensity neutron powder diffraction data collected on Ba 2 MgReO 6 strongly suggests ordering of multipolar moments on Re(VI), likely ferro-octupolar ordering.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Multifunctional Cu 2 TSiS 4 (T = Mn and Fe): Polar Semiconducting Antiferromagnets with Nonlinear Optical Properties

In this work, Cu 2 TSiS 4 (T = Mn and Fe) polycrystalline and single-crystal materials were prepared with high-temperature solid-state and chemical vapor transport methods, respectively. The polar crystal structure (space group Pmn2 1 ) consists of chains of corner-sharing and distorted CuS 4 , Mn/FeS 4 , and SiS 4 tetrahedra, which is confirmed by Rietveld refinement using neutron powder diffraction data, X-ray single-crystal refinement, electron diffraction, energy-dispersive X-ray spectroscopy, and second harmonic generation (SHG) techniques. Magnetic measurements indicate that both compounds order antiferromagnetically at 8 and 14 K, respectively, which is supported by the temperature-dependent (100–2 K) neutron powder diffraction data. Additional magnetic reflections observed at 2 K can be modeled by magnetic propagation vectors k = (1/2,0,1/2) and k = (1/2,1/2,1/2) for Cu 2 MnSiS 4 and Cu 2 FeSiS 4 , respectively. The refined antiferromagnetic structure reveals that the Mn/Fe spins are canted away from the ac plane by about 14°, with the total magnetic moments of Mn and Fe being 4.1(1) and 2.9(1) μ B , respectively. Both compounds exhibit an SHG response with relatively modest second-order nonlinear susceptibilities. Density functional theory calculations are used to describe the electronic band structures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Pressure-Stabilized MnSb2 with Complex Incommensurate Magnetic Order

Marcasite-type compounds have been proposed as promising hosts of exotic magnetic quantum states, yet experimental realizations in stoichiometric, disorder-free systems remain limited. Here, we report the high-pressure stabilization and magnetic characterization of MnSb2, a marcasite-type compound that is thermodynamically metastable under ambient pressure. Single crystals were synthesized using a cubic multianvil press at 3.3 GPa and 490 °C for 24 h, and powder and single-crystal X-ray diffraction confirm the orthorhombic Pnnm structure. These crystals are stable at ambient pressure for a long time up to between 450 and 500 K. Heat-capacity measurements reveal phase transitions at approximately T0 ∼ 118 K and T1 ∼ 220 K. Neutron diffraction uncovers an unconventional magnetic state below T1 ∼ 220 K. Magnetic powder neutron diffraction refinements reveal possible multiple magnetic configurations that provide comparably acceptable fits to the experimental data. While most solutions are consistent with a spin-density-wave (SDW) description, helical models systematically yield inferior agreement factors. Across a broad range of models, the Mn ordered moment reaches a maximum value of approximately 2 μB and remains predominantly collinear, with minimal canting along the c-axis. At 200 K, the magnetic propagation vector is q = (0, 0.3975, 0.3783); upon cooling, the b component increases toward 0.5, reflecting a temperature-dependent evolution of the modulation. The need for modification of the magnetic model between high and low temperatures further highlights the complex and strongly temperature-dependent nature of the magnetic order in this system. These results establish MnSb2 as a pressure-stabilized marcasite magnet with a tunable, complex magnetic state and a compelling stoichiometric platform for exploring unconventional magnetic behavior, including potential altermagnetism.

Xu, Mingyu [Michigan State University , , , ,; Iow↗
DOE OSTI2021

Intertwined Topological and Magnetic Orders in Atomically Thin Chern Insulator MnBi 2 Te 4

The interplay between band topology and magnetic order plays a key role in quantum states of matter. MnBi 2 Te 4 , a van der Waals magnet, has recently emerged as an exciting platform for exploring Chern insulator physics. Its layered antiferromagnetic order was predicted to enable even-odd layer-number dependent topological states, supported by promising edge transport measurements. Furthermore, it becomes a Chern insulator when all spins are aligned by an applied magnetic field. However, the evolution of the bulk electronic structure as the magnetic state is continuously tuned and its dependence on layer number remains unexplored. Here, employing multimodal probes, we establish oneto-one correspondence between bulk electronic structure, magnetic state, topological order, and layer thickness in atomically thin MnBi 2 Te 4 devices. As the magnetic state is tuned through the canted magnetic phase, we observe a band crossing, i.e., the closing and reopening of the bulk bandgap, corresponding to the concurrent topological phase transition. Surprisingly, we find that the even- and odd-layer number devices exhibit a similar topological phase transition coupled to magnetic states, distinct from recent theoretical and experimental reports. Our findings shed new light on the interplay between band topology and magnetic order in this newly discovered topological magnet and validate the band crossing with concurrent measurements of topological invariant in a continuously tuned topological phase transition.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Possible Topological Hall Effect above Room Temperature in Layered Cr 1.2 Te 2 Ferromagnet

Topological Hall effect (THE) has been used as a powerful tool to unlock spin chirality in novel magnetic materials. Recent focus has been widely paid to THE and possible chiral spin textures in two-dimensional (2D) layered magnetic materials. However, the room-temperature THE has been barely reported in 2D materials, which hinders its practical applications in 2D spintronics. In this paper, we report a possible THE signal featuring antisymmetric peaks in a wide temperature window up to 320 K in Cr 1.2 Te 2 , a new quasi-2D ferromagnetic material. The temperature, thickness, and magnetic field dependences of the THE lead to potential spin chirality origin that is associated with the spin canting under external magnetic fields. Furthermore, our work holds promise for practical applications in future chiral spin-based vdW spintronic devices.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

In Situ Local Imaging of Ferromagnetism and Superconductivity in RbEuFe 4 As 4

The coexistence of superconductivity and ferromagnetism is an intrinsically interesting research focus in condensed matter physics but the study is limited by low superconducting (T c ) and magnetic (T m ) transition temperatures in related materials. Here, we used a scanning superconducting quantum interference device to image the in-situ diamagnetic and ferromagnetic responses of RbEuFe 4 As 4 with high T c and T m . We observed significant suppression of superfluid density in vicinity of the magnetic phase transition, signifying fluctuation-enhanced magnetic scatterings between Eu spins and Fe 3d conduction electrons. Intriguingly, we observed multiple ferromagnetic domains which should be absent in an ideal magnetic helical phase. The formation of these domains demonstrates a weak c-axis ferromagnetic component probably arising from Eu spin-canting effect, indicative of possible superconductivity-driven domain Meissner and domain vortex-antivortex phases as revealed in EuFe 2 (As 0.79 P 0.21 ) 2 . Finally, our observations highlight RbEuFe 4 As 4 is a unique system which includes multiple interplay channels between superconductivity and ferromagnetism.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Strain and Defect-Tailored Magnetotransport in NiCo 2 O 4 Thin Films and Freestanding Membranes

Magnetic spinel NiCo 2 O 4 is promising for developing spintronic applications due to its high magnetic Curie temperature, high spin polarization, fast spin dynamics, and strain-tunable magnetic anisotropy, while its electronic and magnetic properties depend sensitively on epitaxial strain and disorder. Here, in this study, we use epitaxial NiCo 2 O 4 thin films and freestanding NiCo 2 O 4 membranes as model systems to reveal the complex interplay of strain and defects in determining the metallicity and magnetotransport properties of the ferrimagnetic spinel. NiCo 2 O 4 on perovskite substrates and NiCo 2 O 4 membranes exhibit insulating behaviors and spin canting, in sharp contrast to the metallic NiCo 2 O 4 films on spinel substrates that possess strong perpendicular magnetic anisotropy. Anisotropic magnetoresistance studies provide critical information about disorder-induced spin scattering and strain-induced tetragonal magnetocrystalline anisotropy, which is corroborated by comprehensive electron microscopy characterizations. Our study presents a promising venue for designing flexible magnetic memory, sensor, and spintronic applications.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Surfactant Removal for Colloidal Nanocrystal Catalysts Mediated by N-Heterocyclic Carbenes

In this work, we report the facile removal of surfactants from col-loidally synthesized nanocrystals via a ligand ex-change with N-heterocyclic carbene (NHC). Subse-quent protonation of the NHC ligand in acid efficient-ly cleans the nanocrystal surface while preserving their uniform morphology and structure for catalysis. The broad efficacy of this strategy is validated using monodisperse Pt, Pd, and Au nanocrystals, each pre-pared with strongly bound phosphine stabilizers. The surface activated nanocrystals exhibit signifi-cantly improved catalytic activities, superior to other surface cleaning methods, as demonstrated in two centrally important electrochemical reactions (glyc-erol oxidation and CO 2 reduction). This work high-lights a new surface activation strategy for catalysis and other applications that enables the efficient use of well-defined nanocrystal libraries prepared by colloidal chemistry.

25 ENERGY STORAGE↗
DOE OSTI2021

The Mechanism of Increasing Summer Water Vapor Over the Tibetan Plateau

Rapid warming over the Tibetan Plateau (TP) has been associated with a wetting trend in atmospheric water vapor content, which is critical for recharging the Asian water tower. However, the mechanism associated with the wetting phenomenon remains unclear. Long-term changes in moisture balance and precipitation recycling processes are investigated using the ERA5 reanalysis from 1979 to 2019. The wetting trend over TP is mainly due to the summer water vapor trend with signi?cantly increases over the western TP. Based on the moisture balance analysis, it is found that precipitation, evaporation, and the convergence of moisture are all increasing over the western TP but decreasing over the eastern TP. Based on the dynamical precipitation recycling model, the results suggest that both internal and external cycles contributes to the wetting over TP, with 63.87% and 36.13% contributions respectively. Further analysis found that the atmospheric heating source is also increasing over the western TP, which could shift the moisture transportation from east to west at the southern boundary of TP. The increasing moisture convergence could enhance precipitation, and the enhanced latent heating in the mid-atmosphere can further induced moisture convergence, which forms a positive feedback. However, an opposite situation occurred over the eastern TP. The internal and external cycle of the recycling process can stimulate (suppress) each other through precipitation over the western (eastern) TP. This mechanism linked the changes in the precipitation recycling and atmospheric circulation, and induced the wetting trend over TP in summer.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Reversible hydrogen control of antiferromagnetic anisotropy in α-Fe 2 O 3

Antiferromagnetic insulators are a ubiquitous class of magnetic materials, holding the promise of low-dissipation spin-based computing devices that can display ultra-fast switching and are robust against stray fields. However, their imperviousness to magnetic fields also makes them difficult to control in a reversible and scalable manner. Here we demonstrate a novel proof-of-principle ionic approach to control the spin reorientation (Morin) transition reversibly in the common antiferromagnetic insulator α-Fe 2 O 3 (haematite) - now an emerging spintronic material that hosts topological antiferromagnetic spin-textures and long magnon-diffusion lengths. We use a low-temperature catalytic-spillover process involving the post-growth incorporation or removal of hydrogen from α-Fe 2 O 3 thin films. Hydrogenation drives pronounced changes in its magnetic anisotropy, Néel vector orientation and canted magnetism via electron injection and local distortions. We explain these effects with a detailed magnetic anisotropy model and first-principles calculations. Tailoring our work for future applications, we demonstrate reversible control of the room-temperature spin-state by doping/expelling hydrogen in Rh-substituted α-Fe 2 O 3 .

36 MATERIALS SCIENCE↗
DOE OSTI2021

Observation of novel charge ordering and spin reorientation in perovskite oxide PbFeO 3

Pb M O 3 ( M = 3 d transition metals) family shows systematic variations in charge distribution and intriguing physical properties due to its delicate energy balance between Pb 6 s and transition metal 3 d orbitals. However, the detailed structure and physical properties of PbFeO 3 remain unclear. Herein, we reveal that PbFeO 3 crystallizes into an unusual 2 a p × 6 a p × 2 a p orthorhombic perovskite super unit cell with space group Cmcm . The distinctive crystal construction and valence distribution of Pb 2+ 0.5 Pb 4+ 0.5 FeO 3 lead to a long range charge ordering of the -A-B-B- type of the layers with two different oxidation states of Pb (Pb 2+ and Pb 4+ ) in them. A weak ferromagnetic transition with canted antiferromagnetic spins along the a -axis is found to occur at 600 K. In addition, decreasing the temperature causes a spin reorientation transition towards a collinear antiferromagnetic structure with spin moments along the b -axis near 418 K. Our theoretical investigations reveal that the peculiar charge ordering of Pb generates two Fe 3+ magnetic sublattices with competing anisotropic energies, giving rise to the spin reorientation at such a high critical temperature.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

An antisite defect mechanism for room temperature ferroelectricity in orthoferrites

Single-phase multiferroic materials that allow the coexistence of ferroelectric and magnetic ordering above room temperature are highly desirable, motivating an ongoing search for mechanisms for unconventional ferroelectricity in magnetic oxides. Here, we report an antisite defect mechanism for room temperature ferroelectricity in epitaxial thin films of yttrium orthoferrite, YFeO 3 , a perovskite-structured canted antiferromagnet. A combination of piezoresponse force microscopy, atomically resolved elemental mapping with aberration corrected scanning transmission electron microscopy and density functional theory calculations reveals that the presence of Y Fe antisite defects facilitates a non-centrosymmetric distortion promoting ferroelectricity. This mechanism is predicted to work analogously for other rare earth orthoferrites, with a dependence of the polarization on the radius of the rare earth cation. Our work uncovers the distinctive role of antisite defects in providing a mechanism for ferroelectricity in a range of magnetic orthoferrites and further augments the functionality of this family of complex oxides for multiferroic applications.

36 MATERIALS SCIENCE↗