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DOE OSTI2023

Magnetic structures and excitations in sawtooth olivine chalcogenides Mn 2 SiX 4 (X = S, Se)

The Mn lattice in olivine chalcogenide Mn 2 SiX 4 (X = S, Se) compounds forms a sawtooth, which is of special interest in magnetism owing to the possibility of realizing flat bands in magnon spectra, a key component in magnonics. In this work, we investigate the Mn 2 SiX 4 olivines using magnetic susceptibility, and X-ray and neutron diffraction. We have determined the average and local crystal structures of Mn 2 SiS 4 and Mn 2 SiSe 4 using synchrotron X-ray, neutron diffraction, and X-ray total scattering data followed by Rietveld and pair distribution function analyses. It is found from the pair distribution function analysis that the Mn triangle that constitutes the sawtooth is isosceles in Mn 2 SiS 4 and Mn 2 SiSe 4 . The temperature evolution of magnetic susceptibility of Mn 2 SiS 4 and Mn 2 SiSe 4 shows anomalies below 83 K and 70 K, respectively, associated with magnetic ordering. From the neutron powder diffraction measurements the magnetic space groups of Mn 2 SiS 4 and Mn 2 SiSe 4 are found to be Pnma and Pnm'a', respectively. Here, we find that the Mn spins adopt a ferromagnetic alignment on the sawtooth in both Mn 2 SiS 4 and Mn 2 SiSe 4 but along different crystallographic directions for the S and the Se compounds. From the temperature evolution of Mn magnetic moments obtained from refining neutron diffraction data, the transition temperatures are accurately determined as T N (S) = 83(2) K and T N (Se) = 70.0(5) K. Broad diffuse magnetic peaks are observed in both the compounds, and are prominently seen close to T N , suggesting the presence of a short-range magnetic order. The magnetic excitations studied using inelastic neutron scattering reveal a magnon excitation with an energy corresponding to approximately 4.5 meV in both S and Se compounds. Spin correlations are observed to persist up to 125 K much above the ordering temperature and we suggest the possibility of short-range spin correlations responsible for this.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

First principles study of nearly strain-free Ni/WSe 2 and Ni/MoS 2 interfaces

Metal/transition metal dichalcogenide interfaces are the subject of active research, in part because they provide various possibilities for interplay of electronic and magnetic properties with potential device applications. Here, we present results of our first principles calculations of nearly strain-free Ni/WSe 2 and Ni/MoS 2 interfaces in thin-film geometry. It is shown that while both the WSe 2 and MoS 2 layers adjacent to Ni undergo metallic transition, the layers farther from the interface remain semiconducting. In addition, a moderate value of spin-polarization is induced on interfacial WSe 2 and MoS 2 layers. At the same time, the electronic and magnetic properties of Ni are nearly unaffected by the presence of WSe 2 and MoS 2 , except a small reduction of magnetic moment at the interfacial Ni atoms. Furthermore, these results can be used as a reference for experimental efforts on epitaxial metal/transition metal dichalcogenide heterostructures, with potential application in modern magnetic storage devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2017

Filling the holes in the CaFe 4 As 3 structure: Synthesis and magnetism of CaCo 5 As 3

Here, we investigate single crystals of CaCo 5 As 3 by means of single-crystal x-ray diffraction, microprobe, magnetic susceptibility, heat capacity, and pressure-dependent transport measurements. CaCo 5 As 3 shares the same structure of CaFe 4 As 3 with an additional Co atom filling a lattice vacancy and undergoes a magnetic transition at T M = 16 K associated with a frustrated magnetic order. CaCo 5 As 3 displays metallic behavior and its Sommerfeld coefficient (γ = 70 mJ/mol K 2 ) indicates a moderate enhancement of electron-electron correlations. Transport data under pressures to 2.5 GPa reveal a suppression of T M at a rate of - 0.008 K/GPa. First-principles electronic structure calculations show a complex three-dimensional band structure and magnetic moments that depend on the local environment at each Co site. Our results are compared with previous data on CaFe 4 As 3 and provide a scenario for a magnetically frustrated ground state in this family of compounds.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2021

Magnetic Compton Scattering Study of Li-Rich Battery Materials

The redox process in a lithium-ion battery occurs when a conduction electron from the lithium anode is transferred to the redox orbital of the cathode. Understanding the nature of orbitals involved in anionic as well as cationic redox reactions is important for improving the capacity and energy density of Li-ion batteries. In this connection, we have obtained magnetic Compton profiles (MCPs) from the Li-rich cation-disordered rock-salt compound LixTi0.4Mn0.4O2 (LTMO). The MCPs, which involved the scattering of circularly polarized hard X-rays, are given by the momentum density of all the unpaired spins in the material. The net magnetic moment in the ground state can be extracted from the area under the MCP, along with a SQUID measurement. Our analysis gives insight into the role of Mn 3d magnetic electrons and O 2p holes in the magnetic redox properties of LTMO.

Suzuki, Kosuke (ORCID:0000000317110604)↗

NASA NTRS1977

The magnetic field of Mercury

The Mariner 10 spacecraft encountered Mercury three times in 1974-1975. The first and third encounters provided detailed observations of a well-developed detached bow shock wave which results from the interaction of the solar wind. The planet possesses a global magnetic field and a modest magnetosphere, which deflects the solar wind. The field is approximately dipolar, with orientation in the same sense as earth, tilted 12 deg from the rotation axis. The magnetic moment corresponds to an undistorted equatorial field intensity of 350 gammas, approximately 1% of earth's. The field, while unequivocally intrinsic to the planet, may be due to remanent magnetization acquired from an extinct dynamo or a primordial magnetic field or due to a presently active dynamo. The latter possibility appears more plausible at present. In any case, the existence of the magnetic field provides very strong evidence of a mature differentiated planetary interior with a large core (core radius about 0.7 Mercury radius) and a record of the history of planetary formation in the magnetization of the crustal rocks.

Ness, N. F.↗

NASA NTRS2013

Computational Studies of Magnetic Nozzle Performance

An extensive literature review of magnetic nozzle research has been performed, examining previous work, as well as a review of fundamental principles. This has allow us to catalog all basic physical mechanisms which we believe underlie the thrust generation process. Energy conversion mechanisms include the approximate conservation of the magnetic moment adiabatic invariant, generalized hall and thermoelectric acceleration, swirl acceleration, thermal energy transformation into directed kinetic energy, and Joule heating. Momentum transfer results from the interaction of the applied magnetic field with currents induced in the plasma plume., while plasma detachment mechanisms include resistive diffusion, recombination and charge exchange collisions, magnetic reconnection, loss of adiabaticity, inertial forces, current closure, and self-field detachment. We have performed a preliminary study of Hall effects on magnetic nozzle jets with weak guiding magnetic fields and weak expansions (p(sub jet) approx. = P(sub background)). The conclusion from this study is that the Hall effect creates an azimuthal rotation of the plasma jet and, more generally, creates helical structures in the induced current, velocity field, and magnetic fields. We have studied plasma jet expansion to near vacuum without a guiding magnetic field, and are presently including a guiding magnetic field using a resistive MHD solver. This research is progressing toward the implementation of a full generalized Ohm's law solver. In our paper, we will summarize the basic principle, as well as the literature survey and briefly review our previous results. Our most recent results at the time of submittal will also be included. Efforts are currently underway to construct an experiment at the University of Michigan Plasmadynamics and Electric Propulsion Laboratory (PEPL) to study magnetic nozzle physics for a RF-thruster. Our computational study will work directly with this experiment to validate the numerical model, in order to study magnetic nozzle physics and optimize magnetic nozzle design. Preliminary results from the PEPL experiment will also be presented.

Ebersohn, Frans H.↗

DOE OSTI2017

Low temperature magnetic structure of CeRhIn 5 by neutron diffraction on absorption-optimized samples

Here, two aspects of the ambient pressure magnetic structure of heavy fermion material CeRhIn 5 have remained under some debate since its discovery: whether the structure is indeed an incommensurate helix or a spin density wave, and what is the precise magnitude of the ordered magnetic moment. By using a single crystal sample optimized for hot neutrons to minimize neutron absorption by Rh and In, here we report an ordered moment of $m=0.54(2)\,{{\mu}_{\text{B}}}$. In addition, by using spherical neutron polarimetry measurements on a similar single crystal sample, we have confirmed the helical nature of the magnetic structure, and identified a single chiral domain.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Hybrid and Inorganic Vacancy-Ordered Double Perovskites A 2 WCl 6

We report hybrid and all-inorganic, vacancy-ordered double perovskites of d 2 W 4+ with the formula A 2 WCl 6 (A = CH 3 NH 3 + , Rb + , and Cs + ). These compounds, which are reddish in color, can be distinguished from structurally similar compounds obtained by hydrothermal methods on the basis of structure, spectroscopic, and magnetic properties. The latter are green and incorporate oxygen, with the actual formula Cs 2 WO x Cl 6–x and distinct optical absorption and emission behavior. Furthermore, the local-moment magnetism of the pure-red d 2 compounds reported here does not correspond to the appropriate Kotani model, suggesting as-yet undiscovered physics in these systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Consequences and Control of Multiscale Order/Disorder in Chiral Magnetic Textures

Transition metal intercalated transition metal dichalcogenides (TMDs) are promising platforms for next-generation spintronic devices based on their wide range of electronic and magnetic phases, which can be tuned by varying the host lattice or intercalant’s identity, stoichiometry, or spatial order. Some of these compounds host a chiral magnetic phase in which the helical winding of magnetic moments propagates along a high-symmetry crystalline axis. Previous studies have demonstrated that variation in intercalant concentrations can have a dramatic effect on the formation of chiral domains and ensemble magnetic properties. However, a systematic and comprehensive study of how atomic-scale order and disorder impact these chiral magnetic textures is so far lacking. Here, we leverage a combination of imaging modes in the (scanning) transmission electron microscope (S/TEM) to directly probe (dis)order across multiple length scales and show how subtle changes in the atomic lattice can tune the mesoscale spin textures and bulk magnetic response in Cr 1/3 NbS 2 , with direct implications for the fundamental understanding and technological implementation of such compounds.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Trimer-based spin liquid candidate B a 4 NbI r 3 O 12

Ba 4 NbIr 3 O 12 , a material with a triangular planar geometry of Ir 3 O 12 trimers, is described. Magnetic susceptibility measurements show it to be paramagnetic with no magnetic ordering down to 1.8 K despite the Curie-Weiss temperature (θ CW ) of -13 K. The material has a very low effective magnetic moment (μeff) of 0.80 μ B /f.u. To look at the lower-temperature behavior, the specific heat (C p ) was measured down to 0.35 K; it shows no indication of magnetic ordering and fitting a power law to C p vs T below 2 K yields the power α = 3/4. Comparison to the trimer compound made with the 4d element Rh in place of the 5d element Ir, Ba 4 NbRh 3 O 12 , which is also paramagnetic (μ eff = 1.48μ B /f.u., θ CW = -23K), is presented. Furthermore, the analysis suggests that Ba 4 NbIr 3 O 12 is a candidate spin liquid material.

36 MATERIALS SCIENCE↗

NASA NTRS2016

Magnetic Shield Design Modeling and Validation for SWOT Spacecraft Ka-Band Extended Interaction Klystron

Two Extended Interaction Klystrons (EIKs) containing strong permanent magnets were modeled magnetically in a representative spacecraft geometry using commercial finite element modeling techniques and were validated against measurements made at varying distances. Initial modeling results for the 63 A-m2 dipole moment magnets showed that magnetic shields would be necessary in order to meet magnetic field requirements for the Surface Water and Ocean Topography (SWOT) spacecraft, which contains components that are susceptible to external DC magnetic fields. JPL and the EIK vendor proposed cold rolled steel and mu-metal as potential shield materials along with proposed thicknesses of 0.5 mm and 1.5 mm. Magnetic shields made from each of these materials were designed and modeled in software, taking highfield saturation into account. Prototype magnetic shields with these parameters were then built, measured with an existing EIK, and compared against modeling results. For single-axis field measurements along the dipole axis, modeling results were within 7 gauss of the measured values at 10 cm from the magnet, and converged to less than 1.5 gauss at distances greater than 14 cm from the magnet. Three-axis field measurements at locations of interest showed that model correlation improved to within 4 gauss at 11 cm and 2 gauss for distances ranging between 15 cm and 36 cm.

Gonzales, Edward↗

DOE OSTI2021

Interface-driven magnetic anisotropy in relaxed La 0.7 Sr 0.3 CrO 3 /La 0.7 Sr 0.3 MnO 3 heterostructures on MgO

We investigate the structural and magnetic properties of La 0.7 Sr 0.3 CrO 3 /La 0.7 Sr 0.3 MnO 3 (LSMO) heterostructures grown on (001)-oriented MgO by molecular beam epitaxy. Due to the large film-substrate lattice mismatch, strain relaxation is found to occur within the first 2–3 unit cells (uc) of the film as evidenced by reflection high energy electron diffraction and high-resolution synchrotron x-ray reciprocal space mapping. Furthermore, we find that the presence of the LSCO spacer and capping layers leads to ferromagnetism in ultra-thin LSMO layers with thicknesses of the order of 2 uc with the magnetic easy axis oriented in the film plane. Net magnetic moments of 1.4 and 2.4 μ B /Mn are measured for (2 uc LSCO/2 uc LSMO) and (2 uc LSCO/4 uc LSMO) superlattices, respectively, by superconducting quantum interference device magnetometry. The effective magnetic anisotropy of the relaxed (2 uc LSCO/4 uc LSMO) heterostructure is found to be an order of magnitude higher than bulk LSMO highlighting the critical role of interfacial interactions in tuning magnetic anisotropy at complex oxide interfaces.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

Multimodal Approach Reveals the Symmetry-Breaking Pathway to the Broken Helix in EuIn 2 ⁢As 2

Understanding and manipulating emergent phases, which are themes at the forefront of quantum-materials research, rely on identifying their underlying symmetries. This general principle has been particularly prominent in materials with coupled electronic and magnetic degrees of freedom, in which magnetic order influences the electronic band structure and can lead to exotic topological effects. However, identifying symmetry of a magnetically ordered phase can pose a challenge, particularly in the presence of small domains. Here we introduce a multimodal approach for determining magnetic structures, which combines symmetry-sensitive optical probes, scattering, and group-theoretical analysis. We apply it to EuIn 2 ⁢As 2 , a material that has received attention as a candidate axion insulator. While first-principles calculations predict this state on the assumption of a simple collinear antiferromagnetic structure, subsequent neutron-scattering measurements reveal a much more intricate magnetic ground state characterized by two coexisting magnetic wave vectors reached by successive thermal phase transitions. The proposed high- and low-temperature phases are a spin helix and a state with interpenetrating helical and Néel antiferromagnetic order termed a “broken helix,” respectively. Employing a multimodal approach, we identify the magnetic structure associated with these two phases of EuIn 2 ⁢As 2 . We find that the higher-temperature phase is characterized by a variation of the magnetic moment amplitude from layer to layer, with the moment vanishing entirely in every third Eu layer. The lower-temperature structure is similar to the broken helix, with one important difference: Because of local strain, the relative orientation of the magnetic structure and the lattice is not fixed. Consequently, the symmetry required to protect the axion phase is not generically protected in EuIn 2 ⁢As 2 , but we show that it can be restored if the magnetic structure is tuned with uniaxial strain. Finally, we present a spin Hamiltonian that identifies the spin interactions that account for the complex magnetic order in EuIn 2 ⁢As 2 . Our work highlights the importance of a multimodal approach in determining the symmetry of complex order parameters.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

NASA NTRS1985

What we have learned about the magnetic field of Mars

Sufficient and unambiguous evidences of the intrinsic martian magnetic field are: (1) the independence of the field polarity in Maritan magnetic tail from interplanetary magnetic fields (IMF) polarity inversion, established with the help of Mars-5 data; and (2) the incongruity between the sign of the radial component of the field measured in Martian tail (Mars-2) and that of the draped model with IMF data measured simultaneously (Mars-3) on February 23-24, 1972. Mar's dipole magnetic moment is within the limits (1.5 to 2.2) x 10 to e 22 G cc. The dipole axis is deflected from that of rotation on the angle I 15 deg. The North magnetic pole is located in the South Hemisphere. In the frame of the precession-dinamo model the magnetic fields of the planets Mars and Earth are similar. The Martian magnetic field is the real obstacle for the solar wind near the planet.

Dolginov, S. S.↗

DOE OSTI2020

Design and performance of an in-vacuum, magnetic field mapping system for the Muon g-2 experiment

The E989 Muon g-2 experiment at Fermilab aims to measure the anomalous magnetic moment, a$_\mu$, of the muon with a precision of 140 parts-per-billion. This requires a precise measurement of both the anomalous spin precession frequency, $\omega_a$, and the average magnetic field in terms of the equivalent, free proton Larmor frequency, $\omega_p$. The measurement of $\omega_p$ with a total systematic uncertainty of 70 parts-per-billion involves a combination of various NMR probes. There are 378 probes in fixed locations constantly monitoring field drifts. A water-based probe provides the calibration in terms of $\omega_p$. A crucial element for the multi-step measurement of $\omega_p$ is the regular mapping of the magnetic field over the muon storage region. The former E821 experiment at Brookhaven employed an in-vacuum field mapping system equipped with 17 NMR probes, which was developed by the University of Heidelberg. We have refurbished and upgraded this system with new probes and electronics. The upgrades include a new communication scheme incorporating time-division multiplexing to separate the important NMR reference clock from the data communication. The addition digitization of the NMR signals replaced the hardware-implemented zero-crossing counting of the E821 system. The digitized signals offer new capabilities in the NMR frequency analysis and its related systematic uncertainties. While the mechanical systems that move the field mapper around the ring have been mostly refurbished, the motion control system was completely replaced with a custom-built electronics centered around a commercial Galil motion controller. Both the field mapping NMR system and its motion control were successfully commissioned at Fermilab and have been in reliable operation during the first data taking periods. This article provides details of the upgrades of the field mapper and its performance.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2022

Ferromagnetism in Pr-rich binary Pr 7 Ru 3 intermetallic compound

We present the synthesis and experimental characterization of the binary intermetallic compound Pr 7 Ru 3 . The polycrystalline sample was prepared by arc melting pure Pr and Ru, followed by homogenization at 500 °C and 600 °C for 48 and 89 h, respectively. Powder x-ray diffraction confirms that Pr 7 Ru 3 crystallizes in an orthorhombic crystal structure (Pnma, space group no. 62) with the lattice parameters: a = 7.3606(7) Å, b = 23.120(1) Å and c = 6.5959(5) Å. Magnetization, resistivity, and heat capacity measurements reveal a ferromagnetic transition in Pr 7 Ru 3 with the Curie temperature T C ~ 24.5 K. The bulk transition is confirmed by a large λ-shape anomaly observed in the specific heat measurement. The magnetic susceptibility above the transition obeys the modified Curie-Weiss law with a positive Curie-Weiss temperature $\ominus$ CW = 30(1) K and an effective magnetic moment of 3.39(1) μ B /Pr. Resistivity data for Pr 7 Ru 3 reveals metallic-like behavior with a clear anomaly at the transition temperature which is smeared by an applied magnetic field. We also synthesized high-quality nonmagnetic analog La 7 Ru 3 for which superconducting transition is observed with T c = 1.95 K, in agreement with the literature.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Integration of amorphous ferromagnetic oxides with multiferroic materials for room temperature magnetoelectric spintronics

A room temperature amorphous ferromagnetic oxide semiconductor can substantially reduce the cost and complexity associated with utilizing crystalline materials for spintronic devices. We report a new material (Fe 0.66 Dy 0.24 Tb 0.1 ) 3 O 7-x (FDTO), which shows semiconducting behavior with reasonable electrical conductivity (~500 mOhm-cm), an optical band-gap (2.4 eV), and a large enough magnetic moment (~200 emu/cc), all of which can be tuned by varying the oxygen content during deposition. Magnetoelectric devices were made by integrating ultrathin FDTO with multiferroic BiFeO 3 . A strong enhancement in the magnetic coercive field of FDTO grown on BiFeO 3 validated a large exchange coupling between them. Additionally, FDTO served as an excellent top electrode for ferroelectric switching in BiFeO3 with no sign of degradation after ~10 10 switching cycles. RT magneto-electric coupling was demonstrated by modulating the resistance states of spin-valve structures using electric fields.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Persistent exchange splitting in the chiral helimagnet $\mathrm{Cr}_{1/3}\mathrm{NbS}_2$

Here, using high-resolution angle-resolved photoemission spectroscopy and ab initio calculation, we systematically investigate the electronic structure of the chiral helimagnet Cr 1/3 NbS 2 and its temperature evolution. The comparison with NbS 2 suggests that the electronic structure of Cr 1/3 NbS 2 is strongly modified by the intercalation of Cr atoms. Our ab initio calculation, consistent with experimental results, suggests strong hybridization between Nb- and Cr-derived states near the Fermi level. In the chiral helimagnetic state (below the Curie temperature, T c ), we observe exchange splitting of the energy bands crossing the Fermi level, which follows the temperature evolution of the magnetic moment, suggesting a strong interaction between the conduction electrons and Cr spin moments. Interestingly, the exchange splitting persists far above T c with weak temperature dependence, in drastic contrast to the itinerant ferromagnetism described by the Stoner model, indicating the existence of short-range magnetic order. Our results provide important insights into the interplay between the electronic structure and magnetism in Cr 1/3 NbS 2 , which is helpful for understanding the microscopic mechanism of chiral helimagnetic ordering.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗