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DOE OSTI2015

Magnetic materials at finite temperatures: thermodynamics and combined spin and molecular dynamics derived from first principles calculations

We present a unified approach to describe the combined behavior of the atomic and magnetic degrees of freedom in magnetic materials. Using Monte Carlo simulations directly combined with first principles the Curie temperature can be obtained ab initio in good agreement with experimental values. The large scale constrained first principles calculations have been used to construct effective potentials for both the atomic and magnetic degrees of freedom that allow the unified study of influence of phonon-magnon coupling on the thermodynamics and dynamics of magnetic systems. The MC calculations predict the specific heat of iron in near perfect agreement with experimental results from 300K to above Tc and allow the identification of the importance of the magnon-phonon interaction at the phase-transition. Further Molecular Dynamics and Spin Dynamics calculations elucidate the dynamics of this coupling and open the potential for quantitative and predictive descriptions of dynamic structure factors in magnetic materials using first principles-derived simulations.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Excitons in 2D Magnets

Theoretical abilities that we built: In our QSGW formalism, the electronic eigenfunctions are calculated self-consistently in presence of the ladder e-h vertex corrections to the screened Coulomb exchange. Charge and self-energies are recalculated iterated until the desired tolerance is achieved in the one-particle Green's function. Further, to include the multi-determinantal (spin-flip structure of multiplets) nature of many body correlations we combine QSGW with DMFT. Below we explore various classes of strongly correlated magnetic systems where excitons are sufficiently described within either the QSGW or the QSGW +DMFT approach. In the process, we establish the digrammatic requirements for a minimum-sufficient theory for describing excitons in large classes of materials.

2D magnets↗

DOE OSTI2023

Hardware, methodology and applications of 2 + D backscatter Mössbauer spectroscopy with simultaneous x-ray and γ-ray detection

Abstract A unique method is presented for the acquisition and analysis of 57 Fe backscatter Mössbauer spectra with simultaneous detection of the resonant 14.4 keV γ -rays and the characteristic 6.4 keV x-rays, using a custom-built multi-parameter analyser constructed on the basis of commercial analogue to digital converters and high-speed digital latches. The system allows for the simultaneous registration of Doppler-modulation velocities and photon energies, with up to 4096 and 8192 digital channels respectively. This arrangement is in contrast to most related systems, which detect at a single narrow energy window per detector. Samples of arbitrary atomic structure, morphology and surface topography can be studied without altering the setup or the analysis procedure, provided that the samples are at least micrometre sized. The hardware and software that are used to acquire data with minimal dead time are described and the custom and self-contained methods for post-measurement energy discrimination, background correction and velocity-axis folding are discussed. The data are fit using a general Hamiltonian model for the nuclear energy levels of 57 Fe and a quantum mechanical description of the angular momentum coupling is utilised, with consideration of the crystalline and chemical disorder of the sample under examination. Three examples of distinct magnetic systems, with thicknesses ranging from 5 μ m to 6 mm, that were studied using this method are presented, these are: an amorphous CoFeB-based ribbon with ultra-soft coercivity for high-frequency applications, magnetically hard Nd-Fe-B thick films on Si substrates, examined in both as-deposited and annealed states, and a sample from the nickel-rich iron meteorite NWA 6259 that contains the atomically ordered, elevated coercivity, L 1 0 phase of FeNi, tetrataenite. The wide applicability and usefulness of this method is thus demonstrated on three distinct sample morphologies that required little to no surface preparation prior to examination.

Engineering↗

DOE OSTI2017

Ultra-High Field Magnets for X-Ray and Neutron Scattering using High Temperature Superconductors

X-ray and neutron scattering techniques are capable of acquiring information about the structure and dynamics of quantum matter. However, the high-field magnet systems currently available at x-ray and neutron scattering facilities in the United States are limited to fields of 16 tesla (T) at maximum, which precludes applications that require and/or study ultra-high field states of matter. This gap in capability—and the need to address it—is a central conclusion of the 2005 National Academy of Sciences report by the Committee on Opportunities in High Magnetic Field Science. To address this gap, we propose a magnet development program that would more than double the field range accessible to scattering experiments. With the development and use of new ultra-high field–magnets, the program would bring into view new worlds of quantum matter with profound impacts on our understanding of advanced electronic materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2019

Crystal growth, microstructure, and physical properties of SrMnSb 2

We report on the crystal and magnetic structures, magnetic, and transport properties of SrMnSb 2 single crystals grown by the self-flux method. Magnetic susceptibility measurements reveal an antiferromagnetic (AFM) transition at T N = 295(3) K. Above T N , the susceptibility slightly increases and forms a broad peak at T ~ 420 K, which is a typical feature of two-dimensional magnetic systems. Neutron diffraction measurements on single crystals confirm the previously reported C-type AFM structure below T N . Both de Haas-van Alphen (dHvA) and Shubnikov-de Haas (SdH) effects are observed in SrMnSb2 single crystals. Analysis of the oscillatory component by a Fourier transform shows that the prominent frequencies obtained by the two different techniques are practically the same within error regardless of sample size or saturated magnetic moment. Transmission electron microscopy (TEM) reveals the existence of stacking faults in the crystals, which result from a horizontal shift of Sb atomic layers suggesting possible ordering of Sb vacancies in the crystals. Increase of temperature in susceptibility measurements leads to the formation of a strong peak at T ~ 570 K that upon cooling under magnetic field the susceptibility shows a ferromagnetic transition at T C ~ 580 K. Neutron powder diffraction on crushed single-crystals does not support an FM phase above T N . Furthermore, X-ray magnetic circular dichroism (XMCD) measurements of a single crystal at the L 2,3 edge of Mn shows a signal due to induced canting of AFM moments by the applied magnetic field. All evidence strongly suggests that a chemical transformation at the surface of single crystals occurs above 500 K concurrently producing a minute amount of ferromagnetic impurity phase.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Antiferromagnetism in the van der Waals layered spin-lozenge semiconductor CrTe 3

We have investigated the crystallographic, magnetic, and transport properties of the van der Waals bonded, layered compound CrTe 3 on single-crystal and polycrystalline materials. Furthermore, the crystal structure contains layers made up of lozenge-shaped Cr 4 tetramers. Electrical resistivity measurements show the crystals to be semiconducting, with a temperature dependence consistent with a band gap of 0.3 eV. The magnetic susceptibility exhibits a broad maximum near 300 K characteristic of low dimensional magnetic systems. Weak anomalies are observed in the susceptibility and heat capacity near 55 K, and single-crystal neutron diffraction reveals the onset of long-range antiferromagnetic order at this temperature. Strongly dispersive spin waves are observed in the ordered state. Significant magnetoelastic coupling is indicated by the anomalous temperature dependence of the lattice parameters and is evident in structural optimization in van der Waals density functional theory calculations for different magnetic configurations. The cleavability of the compound is apparent from its handling and is confirmed by first-principles calculations, which predict a cleavage energy 0.5 J / m 2 , similar to graphite. Based on our results, CrTe 3 is identified as a promising compound for studies of low dimensional magnetism in bulk crystals as well as magnetic order in monolayer materials and van der Waals heterostructures.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2016

High-performance superconductors for Fusion Nuclear Science Facility

High-performance superconducting magnets play an important role in the design of the next step large-scale, high-field fusion reactors such as the fusion nuclear science facility (FNSF) and the spherical tokamak (ST) pilot plant beyond ITER. Here, Princeton Plasma Physics Laboratory is currently leading the design studies of the FNSF and the ST pilot plant study. ITER, which is under construction in the south of France, utilizes the state-of-the-art low temperature superconducting magnet technology based on the cable-in-conduit conductor design, where over a thousand multifilament Nb 3 Sn superconducting strands are twisted together to form a high-current-carrying cable inserted into a steel jacket for coil windings. We present design options of the high-performance superconductors in the winding pack for the FNSF toroidal field magnet system based on the toroidal field radial build from the system code. For the low temperature superconductor options, the advanced J c Nb 3 Sn RRP strands (J c > 1000 A/mm 2 at 16 T, 4 K) from Oxford Superconducting Technology are under consideration. For the high-temperature superconductor options, the rectangular-shaped high-current HTS cable made of stacked YBCO tapes will be considered to validate feasibility of TF coil winding pack design for the ST-FNSF magnets.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2015

The total position-spread tensor: Spin partition

The Total Position Spread (TPS) tensor, defined as the second moment cumulant of the position operator, is a key quantity to describe the mobility of electrons in a molecule or an extended system. In the present investigation, the partition of the TPS tensor according to spin variables is derived and discussed. It is shown that, while the spin-summed TPS gives information on charge mobility, the spin-partitioned TPS tensor becomes a powerful tool that provides information about spin fluctuations. The case of the hydrogen molecule is treated, both analytically, by using a 1s Slater-type orbital, and numerically, at Full Configuration Interaction (FCI) level with a V6Z basis set. It is found that, for very large inter-nuclear distances, the partitioned tensor growths quadratically with the distance in some of the low-lying electronic states. This fact is related to the presence of entanglement in the wave function. Non-dimerized open chains described by a model Hubbard Hamiltonian and linear hydrogen chains H{sub n} (n ≥ 2), composed of equally spaced atoms, are also studied at FCI level. The hydrogen systems show the presence of marked maxima for the spin-summed TPS (corresponding to a high charge mobility) when the inter-nuclear distance is about 2 bohrs. This fact can be associated to the presence of a Mott transition occurring in this region. The spin-partitioned TPS tensor, on the other hand, has a quadratical growth at long distances, a fact that corresponds to the high spin mobility in a magnetic system.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

Spin texture induced by non-magnetic doping and spin dynamics in 2D triangular lattice antiferromagnet h -Y(Mn,Al)O 3

Novel effects induced by nonmagnetic impurities in frustrated magnets and quantum spin liquid represent a highly nontrivial and interesting problem. A theoretical proposal of extended modulated spin structures induced by doping of such magnets, distinct from the well-known skyrmions has attracted significant interest. Here, we demonstrate that nonmagnetic impurities can produce such extended spin structures in h-YMnO 3 , a triangular antiferromagnet with noncollinear magnetic order. Using inelastic neutron scattering (INS), we measured the full dynamical structure factor in Al-doped h-YMnO 3 and confirmed the presence of magnon damping with a clear momentum dependence. Our theoretical calculations can reproduce the key features of the INS data, supporting the formation of the proposed spin textures. As such, our study provides the first experimental confirmation of the impurity-induced spin textures. It offers new insights and understanding of the impurity effects in a broad class of noncollinear magnetic systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Functionalizing magnet additive manufacturing with in-situ magnetic field source

Additive manufacturing via 3-D printing technologies have become a frontier in materials research, including its application in the development and recycling of permanent magnets. This work addresses the opportunity to integrate magnetic field sources into 3-D printing process in order to enable printing, alignment of anisotropic permanent magnets or magnetizing of magnetic filler materials, without requiring further processing. Specifically, a nonaxisymmetric electromagnet-type field source architecture was designed, modelled, constructed, installed to a fused filament commercial 3-D printer, and tested. The testing was performed by applying magnetic field while printing composite anisotropic Nd-Fe-B + Sm-Fe-N powders bonded in Nylon12 (65 vol.%) and recycled Sm-Co powder bonded in PLA (15 vol.%). Magnetic characterization indicated that the degree-of-alignment of the magnet powders increased both with alignment field strength (controlled by the electric current applied to the magnetizing system) and the printing temperature. Both coercivity and remanence were found to be strongly dependent on the degree-of-alignment, except for printing performed below but near the Curie temperature of Nd-Fe-B (310 ° C). At applied field of 0.15 kOe, Sm-Co and hybrid Nd-Fe-B/Sm-Fe-N printed samples showed degrees-of-alignment of 83 % and 65 %, respectively. The variations in coercivity were consistent with previous observations in bonded magnet materials. This work verifies that integration of magnetic field sources into 3-D printing processes will result in magnetic alignment of particles while ensuring that other advantages of 3-D printing are retained.

3-D printing↗

DOE OSTI2023

Principal Challenges in Toroidal Magnetic Confinement Fusion Systems

Research efforts toward a practical and economical magnetically confined fusion power source have made steady progress over the years. Today, the principal approaches to confining a hot plasma of Deuterium and Tritium ions long enough for a significant frac/on to undergo thermonuclear burn employ toroidal geometries. Such geometries are attractive because charged particles are tightly bound around the field lines, undergoing locally helical orbits as they travel along those lines. In the core regions of the plasma, the field lines have no connection to the material surfaces making up the interior of the vacuum vessel, so that plasma confinement times can be long enough for significant thermonuclear burnup via fusion reactions to take place. For good confinement, the geometry of the field lines must be such that nested field lines (which lie on nested flux surfaces) twist around the toroidal axis (a quasi-circular line that approximately lies in the center of the confined plasma) at rates that vary based on their distance from that axis. The rotational transform (or field line pitch), iota/2π , is defined as the number of poloidal transits per single toroidal transit of a field line on a toroidal flux surface.

42 ENGINEERING↗

DOE OSTI2013

Microstructures, magnetic and electric properties of diluted magnetic semiconductors InTe{sub 1−x} Fe{sub x} (Co{sub x})

Highlights: ► The prepared InTe{sub 0.9}Fe{sub 0.1} was found to be ferromagnetic at room temperature and can be characterized as diluted magnetic semiconductors. ► The presence of staking faults, various types of defects, strained lattice, grain boundaries and the impurity of minor non-magnetic phase were suggested to participate in high temperature ferromagnetism. - Abstract: InTe compound doped by 10% of Fe or Co respectively was synthesized. X-ray diffraction (XRD), transmission electron microscope (TEM), scanning electron microscope (SEM), energy dispersive X-ray (EDX), vibrating sample magnetometer (VSM) and Kiethley electrometer were used for characterizing the prepared samples. XRD show the presence of InTe{sub 0.9}Fe{sub 0.1} or InTe{sub 0.9}Co{sub 0.1} together with minor In{sub 4}Te{sub 3} phase. InTe{sub 0.9}Fe{sub 0.1} is ferromagnetic with high Curie and high blocking temperature, while InTe{sub 0.9}Co{sub 0.1} is antiferromagnetic with two high Neels temperatures. σRT of InTe{sub 0.9}Fe{sub 0.1} and InTe{sub 0.9}Co{sub 0.1} are greater than those of InTe. The higher conductivity is due to the higher carrier's density obtained from the interaction of the sp-d orbitals, of the electric and magnetic system. The presence of In{sub 4}Te{sub 3} minor phase and different kinds of defects are taking major roles in the formation of high Tc ferromagnetism and antiferromagnetism.

36 MATERIALS SCIENCE↗

DOE OSTI2017

The multi-purpose three-axis spectrometer (TAS) MIRA at FRM II

The cold-neutron three-axis spectrometer MIRA is an instrument optimized for low-energy excitations. Its excellent intrinsic $Q$-resolution makes it ideal for studying incommensurate magnetic systems (elastic and inelastic). MIRA is at the forefront of using advanced neutron focusing optics such as elliptic guides, which enable the investigation of small samples under extreme conditions. Another advantage of MIRA is the modular assembly allowing for instrumental adaption to the needs of the experiment within a few hours. The development of new methods such as the spin-echo technique MIEZE is another important application at MIRA. Finally, scientific topics include the investigation of complex inter-metallic alloys and spectroscopy on incommensurate magnetic structures.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Status of the Mu2e experiment

The Mu2e experiment at Fermilab searches for the coherent, neutrino-less conversion of a μ − to e − in the Coulomb field of Al nuclei, that represents one of the cleanest Charged Lepton Flavor Violating (CLFV) processes for exploring Beyond the Standard Model (BSM) physics. Mu2e aims to improve previous sensitivity by four orders of magnitude, with a distinctive signature provided by identifying mono-energetic electrons with energy slightly below the muon rest mass. To reach this goal, the experiment will use the highest intensity pulsed muon beam in the world, with up to 6 × 1 0 9 stopped muons/sec. This is achieved using the Fermilab proton beam and the design and realization of a unique 25 m long superconducting solenoidal system. The high beam intensity relies upon minimizing beam losses in the slow extraction region, indicating an opportunity of using bent crystals for shadowing. A high-resolution straw tracker and a fast CsI crystal calorimeter identify the conversion electron. Both detectors are inserted behind the Stopping Target in the last solenoid section. A Cosmic Ray Veto covers a large part of the solenoids to suppress background produced by cosmic rays. In this paper, we report the details of the experimental layout, the construction status of the magnetic system and detectors, and a short description of the simulation and realization of the bent crystals. Performing crystal channeling in front of the first slow extraction septa will allow beam shadowing and largely reduce beam losses. •Charge Lepton Flavor Violation processes: μ − → e − conversion.•Large Superconducting Solenoid system.•High-Intensity beams•High precision detectors.•Crystal channeling.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2021

Giant topological Hall effect in centrosymmetric tetragonal Mn 2–x Zn x Sb

Topological magnetism typically appears in noncentrosymmetric compounds or compounds with geometric frustration. Here, we report the effective tuning of magnetism in centrosymmetric tetragonal Mn 2–x Zn x Sb by Zn substitution. The magnetism is found to be closely coupled to the transport properties, giving rise to a very large topological Hall effect with fine-tuning of Zn content, which even persists to high temperature (~250K). The further magnetoentropic analysis suggests that the topological Hall effect is possibly associated with topological magnetism. Furthermore, our finding suggests Mn 2–x Zn x S is a candidate material for a centrosymmetric tetragonal topological magnetic system, offering opportunities for studying and tuning spin textures and developing near room temperature spin-based devices.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Octupolar versus Néel Order in Cubic 5d 2 Double Perovskites

We report time-of-flight neutron spectroscopy and neutron and x-ray diffraction studies of the 5 d 2 double perovskite magnets, Ba 2 M OsO 6 ( M = Zn , Mg , Ca ). We find that these materials host antiferromagnetically coupled 5 d 2 Os 6 + ions decorating a face-centered cubic (fcc) lattice and are found to remain cubic down to the lowest temperatures. They all exhibit thermodynamic anomalies consistent with a single phase transition at a temperature T * , and a gapped magnetic excitation spectrum with spectral weight concentrated at wave vectors typical of type-I antiferromagnetic orders. However, while muon spin resonance experiments show clear evidence for time-reversal symmetry breaking below T * , we observe no corresponding magnetic Bragg scattering signal. These results are shown to be consistent with ferro-octupolar symmetry breaking below T * , and are discussed in the context of other 5 d double perovskite magnets and theories of exotic orders driven by multipolar interactions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2015

THE CONFINED X-CLASS FLARES OF SOLAR ACTIVE REGION 2192

The unusually large active region (AR) NOAA 2192, observed in 2014 October, was outstanding in its productivity of major two-ribbon flares without coronal mass ejections. On a large scale, a predominantly north–south oriented magnetic system of arcade fields served as a strong top and lateral confinement for a series of large two-ribbon flares originating from the core of the AR. The large initial separation of the flare ribbons, together with an almost absent growth in ribbon separation, suggests a confined reconnection site high up in the corona. Based on a detailed analysis of the confined X1.6 flare on October 22, we show how exceptional the flaring of this AR was. We provide evidence for repeated energy release, indicating that the same magnetic field structures were repeatedly involved in magnetic reconnection. We find that a large number of electrons was accelerated to non-thermal energies, revealing a steep power-law spectrum, but that only a small fraction was accelerated to high energies. The total non-thermal energy in electrons derived (on the order of 10{sup 25} J) is considerably higher than that in eruptive flares of class X1, and corresponds to about 10% of the excess magnetic energy present in the active-region corona.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2023

Machine learning nonequilibrium electron forces for spin dynamics of itinerant magnets

Abstract We present a generalized potential theory for conservative as well as nonconservative forces for the Landau-Lifshitz magnetization dynamics. Importantly, this formulation makes possible an elegant generalization of the Behler-Parrinello machine learning (ML) approach, which is a cornerstone of ML-based quantum molecular dynamics methods, to the modeling of force fields in adiabatic spin dynamics of out-of-equilibrium itinerant magnetic systems. We demonstrate our approach by developing a deep-learning neural network that successfully learns the electron-mediated exchange fields in a driven s-d model computed from the nonequilibrium Green’s function method. We show that dynamical simulations with forces predicted from the neural network accurately reproduce the voltage-driven domain-wall propagation. Our work also lays the foundation for ML modeling of spin transfer torques and opens a avenue for ML-based multi-scale modeling of nonequilibrium dynamical phenomena in itinerant magnets and spintronics.

36 MATERIALS SCIENCE↗