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At least 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Local order, disorder, and everything in between: using 91 Zr solid-state NMR spectroscopy to probe zirconium-based metal–organic frameworks

Characterization of metal centers in metal–organic frameworks (MOFs) is critical for rational design and further understanding of structure–property relationships. The short-range structure about Zr atoms is challenging to properly elucidate in many Zr MOFs, particularly when local disorder is present. Static 91 Zr solid-state NMR spectra of the seven zirconium MOFs UiO-66, UiO-66-NH 2 , UiO-67, MOF-801, MOF-808, DUT-68 and DUT-69 have been acquired at high magnetic fields of 35.2 T and 19.6 T, yielding valuable information on the local structure, site symmetry and order about Zr. 91 Zr NMR is very sensitive to differences in MOF short-range structure caused by guest molecules, linker substitution and post-synthetic treatment. Complementary density functional theory (DFT) calculations assist in the interpretation and assignment of 91 Zr solid-state NMR spectra, lend insight into structural origins of 91 Zr NMR parameters and enable determination of local Zr coordination environments. This approach can be extended to many other materials containing zirconium.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Local aging effects in PuB 4 : Growing inhomogeneity and slow dynamics of local field fluctuations probed by 239 Pu NMR

Plutonium-based correlated electron materials host exotic physical phenomena ranging from unconventional heavy-fermion superconductivity to topological Kondo insulating states. Self-irradiation damage can influence many properties of such radioactive materials. Structural disorder effects due to α radiation have been frequently studied using techniques such as transport, thermodynamics, and x-ray diffraction. Here, in this study, we use 239 Pu nuclear magnetic resonance (NMR) to study the long-term influence of self-damage on the lattice and local electronic structures in a single crystal of the candidate topological insulator plutonium tetraboride (PuB 4 ). We first characterize the anisotropy of the 239 Pu resonance and confirm the local axial-site symmetry inferred from previous polycrystalline measurements. Aging effects are then evaluated over the time frame of six years. We find that, though the static 239 Pu NMR spectra show a slight modulation in their shape, their field-rotation pattern reveals no change in 239 Pu local site symmetry over time, suggesting that aging has a surprisingly small impact on the spatial distribution of the static hyperfine field. Further, ligand-site 11 B NMR finds little time-dependent change in the size of electric field gradient around 11 B sites. By contrast, aging has a prominent impact on the 239 Pu NMR relaxation processes and signal intensity. Specifically, aging-induced damage manifests itself as an increase in the spin-lattice relaxation time 𝑇 1 , an increased distribution of 𝑇 1 , and a signal intensity that decreases linearly by 20% per year. An effective spin-spin relaxation time 𝑇 2,eff in the aged sample shortens drastically towards lower temperature, suggesting growth of slow fluctuations of the hyperfine field that are linked to radiation-damage-induced inhomogeneity. Our NMR study sheds light on the interplay of radiation damage and local magnetic interactions in correlated insulators.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Direct Imaging of Resonant Phonon-Magnon Coupling

Detection of phonons is critical for research on the interconversion between resonantly coupled magnons and phonons. Here we report the direct visualization of the resonant coupling of magnons and phonons by microfocused Brillouin light scattering on the Ni/Li Nb O 3 hybrid heterostructure. The static patterns of surface acoustic wave phonons, originating from the interference between the incident wave ψ 0 (A 0 , k, φ 0 ) and reflected wave ψ 1 (A 1 , - k, φ 1 ), can be modulated by magnetic field due to the magnon-phonon coupling. By analyzing the information of phonons obtained from Brillouin spectroscopy, the properties of the magnon system (Ni film), e.g., ferromagnetic resonance field and resonance linewidth, can be determined. The results provide spatially resolved information about phonon manipulation and detection in a coupled magnon-phonon system.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Dynamical piezomagnetic effect in time-reversal-invariant Weyl semimetals with axionic charge density waves

Charge density waves (CDWs) in Weyl semimetals (WSMs) have been shown to induce an exotic axionic insulating phase in which the sliding mode (phason) of the CDW acts as a dynamical axion field, giving rise to a large positive magnetoconductance. In this work, we predict that dynamical strain can induce a bulk orbital magnetization in time-reversal (TR)-invariant WSMs that are gapped by a CDW. Here, we term this effect the “dynamical piezomagnetic effect” (DPME). Unlike in J. Gooth et al., the DPME introduced in this work occurs in a bulk-constant (i.e., static and spatially homogeneous in the bulk) CDW, and does not rely on fluctuations, such as a phason. By studying the low-energy effective theory and a minimal tight-binding (TB) model, we find that the DPME originates from an effective valley axion field that couples the electromagnetic gauge field with a strain-induced pseudogauge field. In particular, whereas the piezoelectric effects studied in previous works are characterized by 2D Berry curvature, the DPME represents the first example of a fundamentally 3D strain effect originating from the Chern-Simons 3-form. We further find that the DPME has a discontinuous change at a critical value of the phase of the CDW order parameter. We demonstrate that, when there is a jump in the DPME, the surface of the system undergoes a topological quantum phase transition (TQPT), while the bulk remains gapped. Hence, the DPME provides a bulk signature of the boundary TQPT in a TR-invariant Weyl CDW.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Canted antiferromagnetic order and spin dynamics in the honeycomb-lattice compound Tb 2 Ir 3 Ga 9

Here, single-crystal neutron diffraction, inelastic neutron scattering, bulk magnetization measurements, and first-principles calculations are used to investigate the magnetic properties of the honeycomb lattice Tb 2 Ir 3 Ga 9 . While the R ln 2 magnetic contribution to the low-temperature entropy indicates a J eff = 1 / 2 moment for the lowest-energy crystal-field doublet, the Tb 3 + ions form a canted antiferromagnetic structure below 12.5 K. Due to the Dzyaloshinskii-Moriya interactions, the Tb moments in the a b plane are slightly canted towards b with a canted moment of 1.22 μ B per formula unit. A minimal x x z spin Hamiltonian is used to simultaneously fit the spin-wave frequencies along the high-symmetry directions and the field dependence of the magnetization along the three crystallographic axes. Long-range magnetic interactions for both in-plane and out-of-plane couplings up to the second nearest neighbors are needed to account for the observed static and dynamic properties. The z component of the exchange interactions between Tb moments is larger than the x and y components. This compound also exhibits bond-dependent exchange with negligible nearest-neighbor exchange coupling between moments parallel and perpendicular to the 4 f orbitals. Despite the J eff = 1 / 2 moments, the spin Hamiltonian is denominated by a large in-plane anisotropy K z ~ – 1 meV . DFT calculations confirm the antiferromagnetic ground state and the substantial interplane coupling at larger Tb-Tb distances.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Nonergodic dynamics in disorder-free potentials

Highlights: • Dynamics in tilted lattices with harmonic confinement is reviewed. • Both spinless and spinful fermions are analyzed. • Local effective tilt is the relevant parameter for nonergodicity. • Neel or domain wall initial states are studied. • Domains with similar spin orientation act as transport and communication barriers. We review the dynamics of interacting particles in disorder-free potentials concentrating on a combination of a harmonic binding with a constant tilt. We show that a simple picture of an effective local tilt describes a variety of cases. Our examples include spinless fermions (as modeled by Heisenberg spin chain in a magnetic field), spinful fermions as well as bosons that enjoy a larger local on-site Hilbert space. We also discuss the domain-wall dynamics that reveals nonergodic features even for a relatively weak tilt as suggested by Doggen et al. (2020). By adding a harmonic potential on top of the static field we confirm that the surprising regular dynamics is not entirely due to Hilbert space shuttering. It seems better explained by the inhibited transport within the domains of identically oriented spins. Once the spin-1/2 restrictions are lifted as, e.g., for bosons, the dynamics involve stronger entanglement generation. Again for domain wall melting, the effect of the harmonic potential is shown to lead mainly to an effective local tilt.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Dynamic metal-linker bonds in metal–organic frameworks

Metal-linker bonds serve as the “glue” that binds metal ions to multitopic organic ligands in the porous materials known as metal–organic frameworks (MOFs). Despite ample evidence of bond lability in molecular and polymeric coordination compounds, the metal-linker bonds of MOFs were long assumed to be rigid and static. Given the importance of ligand fields in determining the behaviour of metal species, labile bonding in MOFs would help explain outstanding questions about MOF behaviour, while providing a design tool for controlling dynamic and stimuli-responsive optoelectronic, magnetic, catalytic, and mechanical phenomena. Here, in this work, we present emerging evidence that MOF metal-linker bonds exist in dynamic equilibria between weakly and tightly bond conformations, and that these equilibria respond to guest–host chemistry, drive phase change behavior, and exhibit size-dependence in MOF nanoparticles.

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

Invariant regimes of Spencer scaling law for magnetic compression of rotating FRC plasma

Abstract The scaling laws for the magnetic compression of a toroidally rotating field reversed configuration (FRC) have been investigated in this work. The magnetohydrodynamics (MHD) simulations of the magnetic compression on rotating FRCs employing the NIMROD code (Sovinec et al 2004 J. Comput. Phys. 195 355), are compared with the Spencer’s one-dimensional (1D) theory (Spencer et al 1983 Phys. Fluids 26 1564) for a wide range of initial flow speeds and profiles. The toroidal flow can influence the scalings directly through the alteration of the compressional work as also evidenced in the 1D adiabatic model, and indirectly by reshaping the initial equilibrium. However, in comparison to the static initial FRC equilibrium cases, the pressure and the radius scalings remain invariant for the magnetic compression ratio B w 2 / B w 1 up to 6 in presence of the initial equilibrium flow, suggesting a broader applicable regime of the Spencer scaling law for FRC magnetic compression. The invariant scaling has been proven a natural consequence of the conservation of angular momentum of both fluid and magnetic field during the dynamic compression process.

Ma, Yiming↗
DOE OSTI2023

Metal–insulator transition in composition-tuned nickel oxide films

Abstract Thin films of the solid solution Nd 1 − x La x NiO 3 are grown in order to study the expected 0 K phase transitions at a specific composition. We experimentally map out the structural, electronic and magnetic properties as a function of x and a discontinuous, possibly first order, insulator–metal transition is observed at low temperature when x = 0.2. Raman spectroscopy and scanning transmission electron microscopy show that this is not associated with a correspondingly discontinuous global structural change. On the other hand, results from density functional theory (DFT) and combined DFT and dynamical mean field theory calculations produce a 0 K first order transition at around this composition. We further estimate the temperature-dependence of the transition from thermodynamic considerations and find that a discontinuous insulator–metal transition can be reproduced theoretically and implies a narrow insulator–metal phase coexistence with x . Finally, muon spin rotation ( µ SR) measurements suggest that there are non-static magnetic moments in the system that may be understood in the context of the first order nature of the 0 K transition and its associated phase coexistence regime.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Gapless Criterion for Crystals from Effective Axion Field

Gapless criteria that can efficiently determine whether a crystal is gapless or not are particularly useful for identifying topological semimetals. In this work, we propose a sufficient gapless criterion for three-dimensional noninteracting crystals, based on the simplified expressions for the bulk average value of the static axion field. The brief logic is that two different simplified expressions give the same value in an insulator, and thus the gapless phase can be detected by the mismatch of them. We demonstrate the effectiveness of the gapless criterion in the magnetic systems with space groups 26 and 13, where mirror, glide, and inversion symmetries provide the simplified expressions. In particular, the gapless criterion can identify gapless phases that are missed by the symmetry-representation approach, as illustrated by space group 26. Our proposal serves as a guiding principle for future discovery of topological semimetals.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Impact of disorder on dynamics and ordering in the honeycomb-lattice iridate Na 2 IrO 3

Kitaev's honeycomb spin-liquid model and its proposed realization in materials such as α-RuCl 3 , Li 2 IrO 3 , and Na 2 IrO 3 continue to present open questions about how the dynamics of a spin liquid are modified in the presence of non-Kitaev interactions as well as the presence of inhomogeneities. Here we use 23 Na nuclear magnetic resonance to probe both static and dynamical magnetic properties in single-crystal Na 2 IrO 3 . We find that the NMR shift follows the bulk susceptibility above 30 K but deviates from it below; moreover below T N the spectra show a broad distribution of internal magnetic fields. Both of these results provide evidence for inequivalent magnetic sites at low temperature, suggesting inhomogeneities are important for the magnetism. The spin-lattice relaxation rate is isotropic and diverges at T N , suggesting that the Kitaev cubic axes may control the critical quantum spin fluctuations. Finally, in the ordered state, we observe gapless excitations, which may arise from site substitution, emergent defects from milder disorder, or possibly be associated with nearby quantum paramagnetic states distinct from the Kitaev spin liquid.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Ultrastrong magnon-magnon coupling and chiral spin-texture control in a dipolar 3D multilayered artificial spin-vortex ice

Strongly-interacting nanomagnetic arrays are ideal systems for exploring reconfigurable magnonics. They provide huge microstate spaces and integrated solutions for storage and neuromorphic computing alongside GHz functionality. These systems may be broadly assessed by their range of reliably accessible states and the strength of magnon coupling phenomena and nonlinearities. Increasingly, nanomagnetic systems are expanding into three-dimensional architectures. This has enhanced the range of available magnetic microstates and functional behaviours, but engineering control over 3D states and dynamics remains challenging. Here, we introduce a 3D magnonic metamaterial composed from multilayered artificial spin ice nanoarrays. Comprising two magnetic layers separated by a non-magnetic spacer, each nanoisland may assume four macrospin or vortex states per magnetic layer. This creates a system with a rich 16 N microstate space and intense static and dynamic dipolar magnetic coupling. The system exhibits a broad range of emergent phenomena driven by the strong inter-layer dipolar interaction, including ultrastrong magnon-magnon coupling with normalised coupling rates of $\frac{Δf}{v}$ = 0.57, GHz mode shifts in zero applied field and chirality-control of magnetic vortex microstates with corresponding magnonic spectra.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Overview of Electrically Conductive and Active Shielding for Wireless Power Transfer with a Polyphase Wireless Electric Vehicle Charging Study

The development and deployment of wireless power transfer (WPT) is increasing across industries including applications in healthcare, sensing and telecommunications, and electric vehicle charging due to its increased mobility and convenience. An important aspect of wireless power transfer is shielding to limit the intensity of electromagnetic fields (EMF) within external regions to protect users and nearby technology. Within this paper, the classifications and recent developments in shielding technologies are reviewed with discussion on potential benefits and drawbacks towards application for wireless charging of electric vehicles (EV). Additionally, a design study is proposed and simulated in 3D FEA for a novel active shield to substantially reduce magnetic field emissions of a high-power, high-frequency rotating-field 3-phase electromagnetic coupler for quickly charging electric vehicles. The active shield, designed to reduce Z-axis emissions, was found to be highly effective, reducing maximum EMF emissions by 83% in aligned static operation and by 50% with lateral misalignment. Active shielding was also found to strongly mitigate the impact of lateral misalignment at each studied partial alignment.

Lewis, Donovin D.↗
DOE OSTI2020

Multiphase magnetism in Yb 2 Ti 2 O 7

We use neutron scattering to show that ferromagnetism and antiferromagnetism coexist in the low T state of the pyrochlore quantum magnet Yb 2 Ti 2 O 7 . While magnetic Bragg peaks evidence long-range static ferromagnetic order, inelastic scattering shows that short-range correlated antiferromagnetism is also present. Small-angle neutron scattering provides direct evidence for mesoscale magnetic structure that we associate with metastable antiferromagnetism. Classical Monte Carlo simulations based on exchange interactions inferred from ⟨ 111 ⟩ -oriented high-field spin wave measurements confirm that antiferromagnetism is metastable within the otherwise ferromagnetic ground state. The apparent lack of coherent spin wave excitations and strong sensitivity to quenched disorder characterizing Yb 2 Ti 2 O 7 is a consequence of this multiphase magnetism.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Trigonal Bipyramidal V 3+ Complex as an Optically Addressable Molecular Qubit Candidate

Synthetic chemistry enables a bottom-up approach to quantum information science, where atoms can be deterministically positioned in a quantum bit or qubit. Two key requirements to realize quantum technologies are qubit initialization and read-out. By imbuing molecular spins with optical initialization and readout mechanisms, analogous to solid-state defects, molecules could be integrated into existing quantum infrastructure. To mimic the electronic structure of optically addressable defect sites, we designed the spin-triplet, V 3+ complex, (C 6 F 5 ) 3 trenVCN t Bu (1).We measured the static spin properties as well as the spin coherence time of1demonstrating coherent control of this spin qubit with a 240 GHz electron paramagnetic resonance spectrometer powered by a free electron laser. We found that1exhibited narrow, near-infrared photoluminescence (PL) from a spin-singlet excited state. Using variable magnetic field PL spectroscopy, we resolved emission into each of the ground-state spin sublevels, a crucial component for spin-selective optical initialization and readout. This work demonstrates that trigonally symmetric, heteroleptic V 3+ complexes are candidates for optical spin addressability.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2022

Inverse Faraday effect in Mott insulators

The inverse Faraday effect (IFE), where a static magnetization is induced by circularly polarized light, offers a promising route to ultrafast control of spin states. Here we study the IFE in Mott insulators using the Floquet theory. We find two distinct IFE behavior governed by the inversion symmetry. In the Mott insulators with inversion symmetry, we find that the effective magnetic field induced by the IFE couples ferromagnetically to the neighboring spins. While for the Mott insulators without inversion symmetry, the effective magnetic field due to IFE couples antiferromagnetically to the neighboring spins. We apply the theory to the spin-orbit coupled single- and multiorbital Hubbard model that is relevant for the Kitaev quantum spin liquid material and demonstrate that the magnetic interactions can be tuned by light.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Effects of external kink and fishbone-like modes on energetic particle transport in tokamak plasmas

Transport and loss of beam injected energetic particles (EPs) due to three-dimensional perturbations, associated with the external kink (XK) instability and fishbone-like mode (FLM), are numerically investigated utilizing the guiding center following code ORBIT for static toroidal plasmas in HL-2A. The perturbation structure for the XK is computed by the MARS-F code and then mapped to the Boozer coordinates as defined in ORBIT. The simulation shows that the EP profile experiences a significant change in the middle of the plasma column, when the XK-induced radial magnetic field perturbation amplitude, normalized by the equilibrium field, exceeds a threshold value of about 10 -2 . The EP transport is found to be dominated by a diffusion process instead of convection. Furthermore, by scanning the perturbation frequency as a free parameter while maintaining the XK mode structure (thus mimicking the FLM as observed in DIII-D and JT-60U tokamaks), redistribution and loss of EPs are found to be substantially enhanced due to strong resonances between the FLM and EPs, when the mode frequency exceeds a threshold value of ~2 kHz for the case considered. For either XK or FLM, the response of passing EPs to the perturbation is dominant due to the assumed tangential neutral beam injection. Most lost EPs due to these instabilities are initially passing particles but are eventually lost through trapped orbits.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Bulk and Nanocrystalline Cesium Lead-Halide Perovskites as Seen by Halide Magnetic Resonance

Lead-halide perovskites increasingly mesmerize researchers because they exhibit a high degree of structural defects and dynamics yet nonetheless offer an outstanding (opto)electronic performance on par with the best examples of structurally stable and defect-free semiconductors. This highly unusual feature necessitates the adoption of an experimental and theoretical mindset and the reexamination of techniques that may be uniquely suited to understand these materials. Surprisingly, the suite of methods for the structural characterization of these materials does not commonly include nuclear magnetic resonance (NMR) spectroscopy. The present study showcases both the utility and versatility of halide NMR and NQR (nuclear quadrupole resonance) for probing the structure and structural dynamics of CsPbX 3 (X = Cl, Br, I), in both bulk and nanocrystalline forms. The strong quadrupole couplings, which originate from the interaction between the large quadrupole moments of, e.g., the 35 Cl, 79 Br, and 127 I nuclei, and the local electric-field gradients, are highly sensitive to subtle structural variations, both static and dynamic. The quadrupole interaction can resolve structural changes with accuracies commensurate with synchrotron X-ray diffraction and scattering. It is shown that space-averaged site-disorder is greatly enhanced in the nanocrystals compared to the bulk, while the dynamics of nuclear spin relaxation indicates enhanced structural dynamics in the nanocrystals. The findings from NMR and NQR were corroborated by ab initio molecular dynamics, which point to the role of the surface in causing the radial strain distribution and disorder. These findings showcase a great synergy between solid-state NMR or NQR and molecular dynamics simulations in shedding light on the structure of soft lead-halide semiconductors.

36 MATERIALS SCIENCE↗