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At least 289 records · Page 16
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Organo‐Functionalized Lacunary Double Cubane‐Type Oxometallates: Synthesis, Structure, and Properties of [(M II Cl) 2 (V IV O) 2 {((HOCH 2 CH 2 )(H)N(CH 2 CH 2 O))(HN(CH 2 CH 2 O) 2 )} 2 ] (M=Co, Zn)

Abstract Organofunctionalized tetranuclear clusters [(M II Cl) 2 (V IV O) 2 {((HOCH 2 CH 2 )(H)N(CH 2 CH 2 O))(HN(CH 2 CH 2 O) 2 )} 2 ] (1, M=Co,2: M=Zn) containing an unprecedented oxometallacyclic {M 2 V 2 Cl 2 N 4 O 8 } (M=Co, Zn) framework have been prepared by solvothermal reactions. The new oxo‐alkoxide compounds were fully characterized by spectroscopic methods, magnetic susceptibility measurement, DFT and ab initio computational methods, and complete single‐crystal X‐ray diffraction structure analysis. The isostructural clusters are formed of edge‐sharing octahedral {VO 5 N} and trigonal bipyramidal {MO 3 NCl} units. Diethanolamine ligates the bimetallic lacunary double cubane core of1and2in an unusual two‐mode fashion, unobserved previously. In the crystalline state, the clusters of1and2are joined by hydrogen bonds to form a three‐dimensional network structure. Magnetic susceptibility data indicate weakly antiferromagnetic interactions between the vanadium centers [J iso (V IV −V IV )=−5.4(1); −3.9(2) cm −1 ], and inequivalent antiferromagnetic interactions between the cobalt and vanadium centers [J iso (V IV −Co II )=−12.6 and −7.5 cm −1 ] contained in1.

Chemistry↗
DOE OSTI2023

Unveiling the Liquid Electrolyte Solvation Structure by Small Angle X-ray Scattering

The fundamental understanding of the liquid electrolyte (LE) solvation structure and electrode–electrolyte interface behavior will bring more in-depth thinking and revolutionary changes to the entire electrochemical energy storage field. Regardless of the variety of techniques available, the methods employed to investigate electrolyte solvation structures over a long-range are severely limited. Small-angle X-ray scattering (SAXS) is an ideal complement to Raman spectroscopy, Fourier transform infrared spectroscopy, or nuclear magnetic resonance, which offers a unique perspective from a larger scale on clusters or networks in electrolytes. Understanding the solvation structures from a few angstroms to hundreds of nanometers will undoubtedly lay a good foundation for studying the macroscopic transport properties, such as viscosity and ionic conductivity, of the LEs. Here, in this Perspective, we discuss the use of SAXS to investigate the solvation structures in different electrolyte systems, a prospect for the SAXS broader application in the electrolyte study, and some challenges that need to be solved in the SAXS application.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

High-Resolution XFEL Structure of the Soluble Methane Monooxygenase Hydroxylase Complex with its Regulatory Component at Ambient Temperature in Two Oxidation States

Soluble methane monooxygenase (sMMO) is a multicomponent metalloenzyme that catalyzes the conversion of methane to methanol at ambient temperature using a nonheme, oxygen-bridged dinuclear iron cluster in the active site. Structural changes in the hydroxylase component (sMMOH) containing the diiron cluster caused by complex formation with a regulatory component (MMOB) and by iron reduction are important for the regulation of O 2 activation and substrate hydroxylation. Structural studies of metalloenzymes using traditional synchrotron-based X-ray crystallography are often complicated by partial X-ray-induced photoreduction of the metal center, thereby obviating determination of the structure of the enzyme in pure oxidation states. Here, microcrystals of the sMMOH:MMOB complex from Methylosinus trichosporium OB3b were serially exposed to X-ray free electron laser (XFEL) pulses, where the ≤35 fs duration of exposure of an individual crystal yields diffraction data before photoreduction-induced structural changes can manifest. Merging diffraction patterns obtained from thousands of crystals generates radiation damage-free, 1.95 Å resolution crystal structures for the fully oxidized and fully reduced states of the sMMOH:MMOB complex for the first time. The results provide new insight into the manner by which the diiron cluster and the active site environment are reorganized by the regulatory protein component in order to enhance the steps of oxygen activation and methane oxidation. Furthermore, this study also emphasizes the value of XFEL and serial femtosecond crystallography (SFX) methods for investigating the structures of metalloenzymes with radiation sensitive metal active sites.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2004

Evolutionary Models of Cold, Magnetized, Interstellar Clouds

We modeled the long-term and small-scale evolution of molecular clouds using direct 2D and 3D magnetohydrodynamic (MHD) simulations. This work followed up on previous research by our group under auspices of the ATP in which we studied the energetics of turbulent, magnetized clouds and their internal structure on intermediate scales. Our new work focused on both global and smallscale aspects of the evolution of turbulent, magnetized clouds, and in particular studied the response of turbulent proto-cloud material to passage through the Galactic spiral potential, and the dynamical collapse of turbulent, magnetized (supercritical) clouds into fragments to initiate the formation of a stellar cluster. Technical advances under this program include developing an adaptive-mesh MHD code as a successor to ZEUS (ATHENA) in order to follow cloud fragmentation, developing a shearing-sheet MHD code which includes self-gravity and externally-imposed gravity to follow the evolution of clouds in the Galactic potential, and developing radiative transfer models to evaluate the internal ionization of clumpy clouds exposed to external photoionizing UV and CR radiation. Gammie's work at UIUC focused on the radiative transfer aspects of this program.

Gammie, Charles F.↗
NASA NTRS2006

Solar Wind Excitation of Pc5 Fluctuations in the Magnetosphere and on the Ground

The primary purpose of this paper is to show the strong link between solar wind compressional fluctuations in the 1-8 mHz frequency range and Pc5 fluctuations in the magnetosphere near the magnetopause, at geosynchronous orbit, over the poles, and on the ground. We focus on a time interval in March and April 2002 when there was a favorable alignment of satellites combined with ten high speed solar wind streams. We used the S3C Great Observatory: specifically, ACE and Wind in the solar wind, Geotail near the magnetopause, GOES 8 and 10 at geosynchronous orbit, Cluster over the poles, and CANOPUS/CARISMA ground stations near the footpoints of magnetic field lines connected to either the magnetopause or the GOES satellites. Using four examples and a statistical survey we show that magnetospheric Pc5 fluctuations exist regardless of IMF orientation and for a wide range of speeds and dynamic pressures; the amplitude and power of magnetospheric fluctuations depends primarily on the amplitude and power of solar wind dynamic pressure fluctuations. The driving and response frequency of these geoeffective fluctuations is in the range 0.5 - 4 mHz. The most striking magnetospheric response occurs when the solar wind speed, dynamic pressure, and dynamic pressure fluctuations all increase at approximately the same time, as frequently occurs near the leading edge of high speed streams. We show evidence of oscillating Poynting Flux at the magnetopause determined using Geotail data that both excites a FLR and propagates evanescently inward. These observations suggest that, at least for this time interval at spring equinox, the entry path is from the dayside equatorial magnetopause inward; multiple field line resonances may be excited from the magnetopause to geosynchronous orbit by propagating compressional waves, with the power decreasing inward away from the magnetopause.

Kessel, Ramona L.↗
DOE OSTI2021

Cluster mediated conversion of amorphous Al(OH) 3 to γ-AlOOH

In this work, we report a synthetic pathway by which amorphous Al(OH) 3 is converted to γ-AlOOH through hydrothermal reaction in the presence of water at temperature T = 473 K. X-ray pair distribution function measurements reveal that the initially amorphous Al(OH) 3 possesses a locally γ-Al(OH) 3 -like structure, while nanocrystalline γ-AlOOH precipitates within 1 h of continuous hydrothermal exposure. Solid state nuclear magnetic resonance measurements show that resonant features associated with four- and five-member Al clusters persist through 20 min of hydrothermal treatment, and ultraviolet (UV) spectra mark the onset of UV-induced photoluminescent features characteristic to γ-AlOOH with 10 min of exposure, indicating a coexistence region of γ-Al(OH) 3 -like and γ-AlOOH-like amorphous species. Furthermore, powder x-ray diffraction measurements of desiccated powders reveal that the conversion process takes place in distinct, power law-defined stages with initial γ-AlOOH nucleation occurring within the first 20 min, followed by a ~ 1 h period of rapid grain coarsening and the subsequent onset of Lifshitz-Slyozov-Wagner-like coalescence.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Large adiabatic temperature change and magnetic frustration in triangular lattice antiferromagnet Dy 2 IrSi 3

While previous studies reveal that the formation of polycrystalline R 2 TX 3 (R = rare-earth, T = transition metal, X = p-block element) type compounds with T = Ir and Co is not achievable without deliberate introduction of atomic vacancies of Ir/Co and Si, here we report successful synthesis of Dy 2 IrSi 3 with fully stoichiometric ratio of constituent elements. An antiferromagnetic transition is manifested in the compound at 6.6 K where only about 50 % of Dy spins take part, while the rest remain in highly frustrated state due to edge-sharing triangular lattice geometry. The magnetic frustration is conclusively probed through magnetization, heat capacity and magnetocaloric study and the frustration parameter (f = |θ p |/T N , θ p , T N being Curie-Weiss and Néel temperatures, respectively) in this case is as large as ~ 3. An additional cluster-glass type transition at ~2.8 K observed in this system has likely been originated due to this magnetic frustration. The magnetocaloric effect reveals an adiabatic temperature change of ~7.5 K for 70 kOe magnetic field, which is one of the largest values reported in intermetallic compounds.

36 MATERIALS SCIENCE↗
NASA NTRS1990

ISM stripping from cluster galaxies and inhomogeneities in cooling flows

Analyses of the x ray surface brightness profiles of cluster cooling flows suggest that the mass flow rate decreases towards the center of the cluster. It is often suggested that this decrease results from thermal instabilities, in which denser blobs of gas cool rapidly and drop below x ray emitting temperatures. If the seeds for the thermal instabilities are entropy perturbations, these perturbations must enter the flow already in the nonlinear regime. Otherwise, the blobs would take too long to cool. Here, researchers suggest that such nonlinear perturbations might start as blobs of interstellar gas which are stripped out of cluster galaxies. Assuming that most of the gas produced by stellar mass loss in cluster galaxies is stripped from the galaxies, the total rate of such stripping is roughly M sub Interstellar Matter (ISM) approx. 100 solar mass yr(-1). It is interesting that the typical rates of cooling in cluster cooling flows are M sub cool approx. 100 solar mass yr(-1). Thus, it is possible that a substantial portion of the cooling gas originates as blobs of interstellar gas stripped from galaxies. The magnetic fields within and outside of the low entropy perturbations can help to maintain their identities, both by suppressing thermal conduction and through the dynamical effects of magnetic tension. One significant question concerning this scenario is: Why are cooling flows seen only in a fraction of clusters, although one would expect gas stripping to be very common. It may be that the density perturbations only survive and cool efficiently in clusters with a very high intracluster gas density and with the focusing effect of a central dominant galaxy. Inhomogeneities in the intracluster medium caused by the stripping of interstellar gas from galaxies can have a number of other effects on clusters. For example, these density fluctuations may disrupt the propagation of radio jets through the intracluster gas, and this may be one mechanism for producing Wide-Angle-Tail radio galaxies.

Soker, Noam↗
NASA NTRS1973

On the relation between solar wind structure and solar wind rotational and tangential discontinuities.

Solar wind plasma and magnetic field data were used to identify rotational and tangential discontinuities during the first 40 days of the flight of Mariner 5. Of the 40 rotational discontinuities found, 36 were clustered in three distinct 3- to 6-day intervals. These three intervals were characterized by high solar wind bulk velocities, high magnetic field magnitudes, low densities, high correlation between velocity and magnetic field changes, and the presence of smooth Alfven waves. The rotational discontinuities had magnetic field changes that were generally close to the direction of magnetic field changes for smooth Alfven waves. Although the primary component of these changes was perpendicular to the equatorial plane for both, the radial component for the discontinuities was generally larger. The normals to the tangential discontinuity surfaces strongly preferred a direction near the ecliptic plane and perpendicular to the spiral field direction.

Turner, J. M.↗
DOE OSTI2020

Hopf Solitons in Helical and Conical Backgrounds of Chiral Magnetic Solids

Three-dimensional topological solitons attract a great deal of interest in fields ranging from particle physics to cosmology, but remain experimentally elusive in solid-state magnets. Here we numerically predict magnetic heliknotons, an embodiment of such nonzero-Hopf-index solitons localized in all spatial dimensions while embedded in a helical or conical background of chiral magnets. In this work we describe conditions under which heliknotons emerge as metastable or ground-state localized nonsingular structures with fascinating knots of magnetization field in widely studied materials. We demonstrate magnetic control of three-dimensional spatial positions of such solitons, as well as show how they interact to form moleculelike clusters and possibly even crystalline phases comprising three-dimensional lattices of such solitons with both orientational and positional order. Finally, we discuss both fundamental importance and potential technological utility of magnetic heliknotons.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

In-situ L-TEM observations of dynamics of nanometric skyrmions and antiskyrmions

Nanometer-scale magnetic skyrmions and antiskyrmions exhibit unique dynamical behaviors in response to external stimuli, which are critical for their applications in low-power-consumption spintronic devices. This review discusses recent advancements in in-situ Lorentz transmission electron microscopy (L-TEM) observations of skyrmion and antiskyrmion dynamics, and demonstrates the manipulation and evolution of these textures in various magnetic materials under electric, magnetic, and thermal stimuli. Specifically, the motion tracking of single skyrmions and their clusters, and the deformation and transformation of skyrmions has been demonstrated in chiral helimagnets FeGe, Co 9 Zn 9 Mn 2 , and Co 10 Zn 10 with precise application of electric currents. Skyrmions can undergo dynamic transitions in current-driven skyrmion motions, from pinned states to linear flows, and even exhibit deformation into elliptical shapes, underscoring their topological robustness and dynamic flexibility. In addition, the manipulation of single antiskyrmions and antiskyrmion-lattice phases in (Fe 0.63 Ni 0.3 Pd 0.07 ) 3 P with S 4 symmetry is discussed, highlighting their high mobility and unique sliding capabilities along stripe domains at room temperature, facilitated by nanosecond pulsed electric currents. Finally, the temperature gradient-driven motion and topological transformation of elliptical skyrmions and antiskyrmions in this same material are investigated. In conclusion, the comprehensive insights gained from the L-TEM imaging technique are pivotal in advancing the design and functionality of next-generation skyrmion/antiskyrmion-based spintronic devices.

(Anti)skyrmion↗
NASA NTRS2014

Plasma and Energetic Particle Behaviors During Asymmetric Magnetic Reconnection at the Magnetopause

The factors controlling asymmetric reconnection and the role of the cold plasma population in the reconnection process are two outstanding questions. We present a case study of multipoint Cluster observations demonstrating that the separatrix and flow boundary angles are greater on the magnetosheath than on the magnetospheric side of the magnetopause, probably due to the stronger density than magnetic field asymmetry at this boundary. The motion of cold plasmaspheric ions entering the reconnection region differs from that of warmer magnetosheath and magnetospheric ions. In contrast to the warmer ions, which are probably accelerated by reconnection in the diffusion region near the subsolar magnetopause, the colder ions are simply entrained by 𝐄×𝐁 drifts at high latitudes on the recently reconnected magnetic field lines. This indicates that plasmaspheric ions can sometimes play only a very limited role in asymmetric reconnection, in contrast to previous simulation studies. Three cold ion populations (probably H+, He+, and O+) appear in the energy spectrum, consistent with ion acceleration to a common velocity.

Cluster↗
DOE OSTI2021

Deep-learning-enabled Bayesian inference of fuel magnetization in magnetized liner inertial fusion

Fuel magnetization in magneto-inertial fusion (MIF) experiments improves charged burn product confinement, reducing requirements on fuel areal density and pressure to achieve self-heating. By elongating the path length of 1.01 MeV tritons produced in a pure deuterium fusion plasma, magnetization enhances the probability for deuterium–tritium reactions producing 11.8-17.1 MeV neutrons. Nuclear diagnostics thus enable a sensitive probe of magnetization. Characterization of magnetization, including uncertainty quantification, is crucial for understanding the physics governing target performance in MIF platforms, such as magnetized liner inertial fusion (MagLIF) experiments conducted at Sandia National Laboratories, Z-facility. We demonstrate a deep-learned surrogate of a physics-based model of nuclear measurements. A single model evaluation is reduced from O ( 10 – 100 ) (10–100) CPU hours on a high-performance computing cluster down to O ( 10 – 100 ) (10) ms on a laptop. This enables a Bayesian inference of magnetization, rigorously accounting for uncertainties from surrogate modeling and noisy nuclear measurements. The approach is validated by testing on synthetic data and comparing with a previous study. We analyze a series of MagLIF experiments systematically varying preheat, resulting in the first ever systematic experimental study of magnetic confinement properties of the fuel plasma as a function of fundamental inputs on any neutron-producing MIF platform. We demonstrate that magnetization decreases from B R ∼ 0.2 ~0.5 to B R ∼ 0.2 ~0.2 MG cm as laser preheat energy deposited increases from E preheat ∼ 460 ~460 J to E preheat ∼ 460 ~1.4 kJ. This trend is consistent with 2D LASNEX simulations showing Nernst advection of the magnetic field out of the hot fuel and diffusion into the target liner.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Control of spin dynamics in artificial honeycomb spin-ice-based nanodisks

In this paper, we report the experimental and theoretical characterization of the angular-dependent spin dynamics in arrays of ferromagnetic nanodisks arranged on a honeycomb lattice. The magnetic field and microwave frequency dependence, measured by broadband ferromagnetic resonance, reveal a rich spectrum of modes that is strongly affected by the microstate of the network. Based on symmetry arguments with respect to the external field, we show that certain parts of the ferromagnetic network contribute to the detected signal. A comparison of the experimental data with micromagnetic simulations reveals that different subsections of the lattice predominantly contribute to the high-frequency response of the array. This is confirmed by optical characterizations using microfocused Brillouin light scattering. Furthermore, we find indications that nucleation and annihilation of vortexlike magnetization configurations in the low-field range affect the dynamics, which is different from clusters of ferromagnetic nanoellipses. Our work opens up new perspectives for designing magnonic devices that combine geometric frustration in gyrotropic vortex crystals at low frequencies with magnonic crystals at high frequencies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Magnetic and electron transport properties of Co 2 Si nanomagnets

In this study, magnetotransport and ferromagnetism in thin films of Co 2 Si nanoclusters are investigated experimentally and theoretically. The nanoclusters are fabricated by an inert-gas condensation-type cluster-deposition method and have an average size of 11.3 nm. Unlike the bulk Co 2 Si that exhibits a very weak net magnetic moment only below 10 K, the nanoclusters exhibit room-temperature ferromagnetism with a substantial saturation magnetization. Key features of the system are its closeness to the Stoner transition, magnetic moments induced by spin polarization starting from surface atoms, and nonuniaxial anisotropy associated with the orthorhombic crystal structure of Co 2 Si . A method is introduced to determine the effective anisotropy using the experimental magnetization data of this complex system and its relationship with the two lowest-order nonuniaxial anisotropy constants. On decreasing temperature from 300 K, the nanoclusters show electron-transport properties unusual for a ferromagnetic metal, including an increase of Hall resistivity and a nonmonotonic change of negative magnetoresistance with a peak at around 100 K. The underlying physics is explained on the basis of the large polarization of surface spins and variation in the degree of their misalignments due to temperature-dependent effective anisotropy.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Mechanisms of Skyrmion and Skyrmion Crystal Formation from the Conical Phase

Real-space topological magnetic structures such as skyrmions and merons are promising candidates for information storage and transport. However, the microscopic mechanisms that control their formation and evolution are still unclear. In this work, using in situ Lorentz transmission electron microscopy, we demonstrate that skyrmion crystals (SkXs) can nucleate, grow, and evolve from the conical phase in the same ways that real nanocrystals form from vapors or solutions. More intriguingly, individual skyrmions can also “reproduce” by division in a mitosis-like process that allows them to annihilate SkX lattice imperfections, which is not available to crystals made of mass-conserving particles. Combined string method and micromagnetic calculations show that competition between repulsive and attractive interactions between skyrmions governs particle-like SkX growth, but nonconservative SkX growth appears to be defect mediated. Our results provide insights toward manipulating magnetic topological states by applying established crystal growth theory, adapted to account for the new process of skyrmion mitosis.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Ferromagnetic MnBi 4 Te 7 obtained with low-concentration Sb doping: A promising platform for exploring topological quantum states

The tuning of the magnetic phase, chemical potential, and structure is crucial to observe diverse exotic topological quantum states in Mn Bi 2 Te 4 (Bi 2 Te 3 ) m (m = 0–3). Here we show a ferromagnetic (FM) phase with a chiral crystal structure in Mn (Bi 1–x Sb x ) 4 Te 7 , obtained via tuning the growth conditions and Sb concentration. Unlike previously reported Mn (Bi 1–x Sb x ) 4 Te 7 , which exhibits FM transitions only at high Sb doping levels, our samples show FM transitions (T C = 13.5 K) at 15%–27% doping levels. Furthermore, our single-crystal x-ray-diffraction structure refinements find Sb doping leads to a chiral structure with the space group of P3, contrasted with the centrosymmetric $P\bar{3}m1$ crystal structure of the parent compound MnBi 4 Te 7 . Through angle-resolved photoemission spectroscopy measurements, we also demonstrated that the nontrivial band topology is preserved in the Sb-doped FM samples. Given that the nontrivial band topology of this system remains robust for low Sb doping levels, our success in making FM Mn(Bi 1–x Sb x ) 4 Te 7 with x = 0.15, 0.175, 0.2, and 0.27 paves the way for realizing the predicted topological quantum states, such as the axion insulator and Weyl semimetals. Additionally, we also observed magnetic glassy behavior in both antiferromagnetic MnBi 4 Te 7 and FM Mn (Bi 1–x Sb x )4 Te 7 samples, which we believe originates from cluster spin-glass phases coexisting with long-range antiferromagnetic/FM orders. Further, we have also discussed how the antisite Mn ions impact the interlayer magnetic coupling and how FM interlayer coupling is stabilized in this system.

36 MATERIALS SCIENCE↗