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At least 325 records · Page 18
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

High mobility in a van der Waals layered antiferromagnetic metal

Van der Waals (vdW) materials with magnetic order have been heavily pursued for fundamental physics as well as for device design. Despite the rapid advances, so far, they are mainly insulating or semiconducting, and none of them has a high electronic mobility—a property that is rare in layered vdW materials in general. The realization of a high-mobility vdW material that also exhibits magnetic order would open the possibility for novel magnetic twistronic or spintronic devices. Here, we report very high carrier mobility in the layered vdW antiferromagnet GdTe 3 . The electron mobility is beyond 60,000 cm 2 V –1 s –1 , which is the highest among all known layered magnetic materials, to the best of our knowledge. Among all known vdW materials, the mobility of bulk GdTe 3 is comparable to that of black phosphorus. By mechanical exfoliation, we further demonstrate that GdTe 3 can be exfoliated to ultrathin flakes of three monolayers.

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

Symmetry-correct bonding in density functional theory calculations for delta phase Pu

The long-held conclusion that magnetic order in delta phase Pu makes the structure mechanically unstable in density functional theory calculations is incorrect if the magnetic order is allowed to be non-collinear. The non-collinear 3Q spin structure is intrinsically cubic and makes all structurally equivalent bonds equivalent in their bonding character. Applied to density functional theory calculations on delta phase Pu, the 3Q spin structure results in elastic constants and phonons with the correct symmetry. Finally, the calculated phonon dispersion agrees better with experiment than previous calculations, and the calculated thermal expansion shows the unique behavior seen experimentally: it is negative.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Large spin-driven dielectric response and magnetoelectric coupling in the buckled honeycomb $Fe_4Nb_2O_9$

Here, we present the significant spin-driven dielectric anomaly (~40% drop) and magnetoelectric coupling near the magnetic ordering temperature in single crystal $Fe_4Nb_2O_9$ . By combining neutron and x-ray single crystal diffraction techniques, we unambiguously determined its magnetic symmetry and studied the structural phase transition at $T_S$ = 70 K. The temperature-dependent static dielectric constant is strongly anisotropic, rendering two dielectric anomalies along the $a$ axis in the hexagonal lattice with the first one coupled to the magnetic ordering around $T_N$ = 97 K and the second one accompanying with a first-order structural transition around $T_S$ = 70 K. Below $T_N$, we found that the anomalous dielectric constant is practically proportional to the square of the magnetic moment from neutron diffraction data, indicating that the exchange striction is likely responsible for the strong spin-lattice coupling. Magnetic-field-induced magnetoelectric coupling was observed and is compatible with the determined magnetic structure that is characteristic of antiferromagnetically arranged ferromagnetic chains in the honeycomb plane. We propose that such magnetic symmetry should be immune to external magnetic fields to some extent favored by the freedom of rotation of moments in the honeycomb plane, laying out a promising system to control the magnetoelectric properties by magnetic fields.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Emergence of electric-field-tunable interfacial ferromagnetism in 2D antiferromagnet heterostructures

Van der Waals (vdW) magnet heterostructures have emerged as new platforms to explore exotic magnetic orders and quantum phenomena. Here, we study heterostructures of layered antiferromagnets, CrI 3 and CrCl 3 , with perpendicular and in-plane magnetic anisotropy, respectively. Using magneto-optical Kerr effect microscopy, we demonstrate out-of-plane magnetic order in the CrCl 3 layer proximal to CrI 3 , with ferromagnetic interfacial coupling between the two. Such an interlayer exchange field leads to higher critical temperature than that of either CrI 3 or CrCl 3 alone. We further demonstrate significant electric-field control of the coercivity, attributed to the naturally broken structural inversion symmetry of the heterostructure allowing unprecedented direct coupling between electric field and interfacial magnetism. These findings illustrate the opportunity to explore exotic magnetic phases and engineer spintronic devices in vdW heterostructures.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Coherent helicity-dependent spin-phonon oscillations in the ferromagnetic van der Waals crystal CrI3

Abstract The discovery of two-dimensional systems hosting intrinsic magnetic order represents a seminal addition to the rich landscape of van der Waals materials. CrI 3 is an archetypal example, where the interdependence of structure and magnetism, along with strong light-matter interactions, provides a new platform to explore the optical control of magnetic and vibrational degrees of freedom at the nanoscale. However, the nature of magneto-structural coupling on its intrinsic ultrafast timescale remains a crucial open question. Here, we probe magnetic and vibrational dynamics in bulk CrI 3 using ultrafast optical spectroscopy, revealing spin-flip scattering-driven demagnetization and strong transient exchange-mediated interactions between lattice vibrations and spin oscillations. The latter yields a coherent spin-coupled phonon mode that is highly sensitive to the driving pulse’s helicity in the magnetically ordered phase. Our results elucidate the nature of ultrafast spin-lattice coupling in CrI 3 and highlight its potential for applications requiring high-speed control of magnetism at the nanoscale.

36 MATERIALS SCIENCE↗
DOE OSTI2024

3D Heisenberg universality in the van der Waals antiferromagnet NiPS 3

Van der Waals (vdW) magnetic materials are comprised of layers of atomically thin sheets, making them ideal platforms for studying magnetism at the two-dimensional (2D) limit. These materials are at the center of a host of novel types of experiments, however, there are notably few pathways to directly probe their magnetic structure. We confirm the magnetic order within a single crystal of NiPS 3 and show it can be accessed with resonant elastic X-ray diffraction along the edge of the vdW planes in a carefully grown crystal by detecting structurally forbidden resonant magnetic X-ray scattering. We find the magnetic order parameter has a critical exponent of β ~ 0.36, indicating that the magnetism of these vdW crystals is more adequately characterized by the three-dimensional (3D) Heisenberg universality class. We verify these findings with first-principles density functional theory, Monte-Carlo simulations, and density matrix renormalization group calculations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Topological magnon band structure of emergent Landau levels in a skyrmion lattice

We report the motion of a spin excitation across topologically nontrivial magnetic order exhibits a deflection that is analogous to the effect of the Lorentz force on an electrically charged particle in an orbital magnetic field. We used polarized inelastic neutron scattering to investigate the propagation of magnons (i.e., bosonic collective spin excitations) in a lattice of skyrmion tubes in manganese silicide. For wave vectors perpendicular to the skyrmion tubes, the magnon spectra are consistent with the formation of finely spaced emergent Landau levels that are characteristic of the fictitious magnetic field used to account for the nontrivial topological winding of the skyrmion lattice. This provides evidence of a topological magnon band structure in reciprocal space, which is borne out of the nontrivial real-space topology of a magnetic order.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Magnetic contribution of itinerant electrons to neutron diffraction in the topological antiferromagnet CeAlGe

We report a neutron diffraction study of the magnetic structure of CeAlGe, a candidate topological semimetal that hosts a noncollinear, multi-𝐤 magnetic phase. By measuring both low- and high-momentum-transfer magnetic Bragg peaks within a single experimental setup, we refine a magnetic structure model based solely on localized Ce moments. This model, which differs from that obtained using only high-𝑄 data, quantitatively reproduces the observed intensities, including the (000) zeroth-order magnetic satellites that are especially sensitive to subtle components of the modulation. While a contribution from itinerant electrons to the zeroth satellite cannot be definitively excluded, our analysis reveals no unambiguous evidence for such effects within experimental uncertainty. The refined magnetic structures exhibit topologically nontrivial winding patterns, derived from the fitted magnetic parameters, that support localized, particle-like spin textures with half-integer topological charges. These features provide a natural microscopic origin for the observed topological Hall effect, establishing CeAlGe as a model system where magnetism and topology are intimately linked.

Magnetic coupling↗
DOE OSTI2022

Thermodynamic insights into the intricate magnetic phase diagram of EuAl 4

The tetragonal intermetallic compound EuAl 4 hosts an exciting variety of low-temperature phases. In addition to a charge density wave below 140 K, four ordered magnetic phases are observed below 15.4 K. Recently, a skyrmion phase was proposed based on Hall effect measurements under a c-axis magnetic field. Here, we present a detailed investigation of the phase transitions in EuAl 4 under c-axis magnetic field. Our dilatometry, heat-capacity, DC magnetometry, AC magnetic susceptibility, and resonant ultrasound spectroscopy measurements reveal three magnetic phase transitions not previously reported. The first key result is a detailed H ∥ [001] magnetic phase diagram mapping the seven phases we observe. Second, we identify a high-field phase, phase VII, which directly corresponds to the region were skyrmions have been previously suggested. Our results provide guidance for future studies exploring the complex magnetic interactions and spin structures in EuAl 4 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Phase diagram of CeSb 2 from magnetostriction and magnetization measurements: Evidence for ferrimagnetic and antiferromagnetic states

Cerium diantimonide (CeSb 2 ) is one of a family of rare-earth-based magnetic materials that exhibit metamagnetism, enabling control of the magnetic ground state through an applied magnetic field. At low temperatures, CeSb 2 hosts a rich phase diagram with multiple magnetically ordered phases for many of which the order parameter is only poorly understood. In this work, we report a study of its metamagnetic properties by scanning tunneling microscopy (STM) and magnetization measurements. We use STM measurements to characterize the sample magnetostriction with subpicometer resolution from magnetic field and temperature sweeps. This allows us to directly assess the bulk phase diagram as a function of field and temperature and relate spectroscopic features from tunneling spectroscopy to bulk phases. Our magnetostriction and magnetization measurements indicate that the low-temperature ground state at zero field is ferrimagnetic. Quasiparticle interference mapping shows evidence for a reconstruction of the electronic structure close to the Fermi energy upon entering the magnetically ordered phase.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Frustrated spin-1/2 dimer compound K 2 Co 2 ( Se O 3 ) 3 with easy-axis anisotropy

Magnetic susceptibility, magnetization, and specific-heat measurements under both in-plane and out-of-plane field on K 2 Co 2 (SeO 3 ) 3 single crystals are reported. The Co dimers in this compound, which are made from face-sharing effective spin-1/2 CoO 6 octahedra, sit on the corners of a geometrically frustrating triangular planar lattice. No long-range magnetic ordering is found down to 0.35 K, which, together with the large negative Curie-Weiss temperature obtained from fitting the temperature-dependent magnetic susceptibility, indicates that the system is magnetically frustrated. Analysis of the field and orientation dependence of the magnetic and thermodynamic properties suggests the presence of an easy-axis anisotropy. Furthermore, the magnetic fluctuations present due to geometric frustration are more resistant to an in-plane field than a perpendicular-to-plane field.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Microscopic Phase Diagram of Eu(Fe 1-x Ni x )As 2 ( x = 0,0.04) Under Pressure

This study will go to establish the microscopic P-T phase diagram of recent 112-type iron-pnictides Eu(Fe 1-x Ni x )As- 2 (x = 0,0.04), high-pressure synchrotron Mossbauer spectroscopy experiments in 151 Eu and 57 Fe have been performed. In EuFeAs 2 application of pressure completely suppresses the itinerant electron magnetism from the Fe sublattice and the local-moment magnetism in Eu ions at similar to ~10 and similar to ~11.6 GPa, respectively. High-pressure x-ray diffraction experiments in EuFeAs 2 reveal an anomalous change in the lattice parameters and a discontinuity in volume around 10 GPa, suggesting an isostructural transition at this pressure. With Ni-doping (x = 0.04), a collapse of local magnetic order occurs at similar to ~8GPa, a lower critical pressure compared with the parent compound. In both systems, the suppression of local-moment magnetism is associated with a significant increase of mean valence in Eu ions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Magnetic excitations from the hexagonal spin clusters in the 𝑆 = $\frac{1}{2}$ distorted honeycomb lattice antiferromagnet Cu 2 ⁢(pymca)⁢ 3 ⁢(ClO 4 )

Cu 2 ⁢(pymca) ⁢3 (ClO 4 ) (pymca: pyrimidine-2-carboxylate) consists of a slightly distorted honeycomb lattice of Cu 2+ spins, which shows no long-range magnetic order down to 0.6 K. A magnetization study revealed 1/3 and 2/3 plateau phases [A. Okutani et al., J. Phys. Soc. Jpn. 88, 013703 (2019)], which is not expected for regular honeycomb antiferromagnets. Inelastic neutron scattering experiments were performed using a powder sample to investigate the exchange interactions of this material. The spin excitations from the singlet ground state to the first three triplet states, predicted from the antiferromagnetic hexagonal spin cluster interacting with 3.9 meV, were observed. Using the exact diagonalization methods, the intercluster coupling was estimated from the excitation peak width to be about 20% of the intracluster interaction, which is consistent with the previously reported value. Finally, our exchange path model explains the anisotropic exchange interactions in the distorted honeycomb plane.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS1995

Quaternary borocarbides: New class of intermetallic superconductors

Our recent discovery of superconductivity (SC) in the four-element multiphase Y-Ni-B-C system at an elevated temperature (TC approximately 12 K) has opened up great possibilities of identifying new superconducting materials and generating new physics. Superconductivity with Tc (greater than 20 K) higher than that known so far in bulk intermetallics has been observed in multiphase Y-Pd-B-C and Th-Pd-B-C systems and a family of single phase materials RENi2B2C (RE= Y, rare earth) have been found. Our investigations show YNi2B2C to be a strong coupling hard type-II SC. HC2(T) exhibits an unconventional temperature dependence. Specific heat and magnetization studies reveal coexistence of SC and magnetism in RNi2B2C (R = Ho, Er, Tm) with magnetic ordering temperatures (Tc approximately 8 K, 10.5 K, 11 K and Tm approximately 5 K, approximately 7K, approximately 4 K respectively) that are remarkably higher than those in known magnetic superconductors . Mu-SR studies suggest the possibility of Ni atoms carrying a moment in TmNi2B2C. Resistivity results suggests a double re-entrant transition (SC-normal-SC) in HoNi2B2C. RENi2B2C (RE = Ce, Nd, Gd) do not show SC down to 4.2 K. The Nd- and Gd-compounds order magnetically at approximately 4.5 K and approximately 19.5 K, respectively. Two SC transitions are observed in Y-Pd-B-C (Tc approximately 22 K, approximately 10 K) and in Th-Pd-B-C (Tc approximately 20 K, approximately 14 K) systems, which indicate that there are at least two structures which support SC in these borocarbides. In our multiphase ThNi2B2C we observe SC at approximately 6 K. No SC was seen in multiphase UNi2B2C, UPd2B2C, UOs2Ge2C and UPd5B3C(0.35) down to 4.2 K. Tc in YNi2B2C is depressed by substitutions (Gd, Th and U at Y-sites and Fe, Co at Ni-sites).

Nagarajan, R.↗
DOE OSTI2023

Hyperbolic exciton polaritons in a van der Waals magnet

Abstract Exciton polaritons are quasiparticles of photons coupled strongly to bound electron-hole pairs, manifesting as an anti-crossing light dispersion near an exciton resonance. Highly anisotropic semiconductors with opposite-signed permittivities along different crystal axes are predicted to host exotic modes inside the anti-crossing called hyperbolic exciton polaritons (HEPs), which confine light subdiffractionally with enhanced density of states. Here, we show observational evidence of steady-state HEPs in the van der Waals magnet chromium sulfide bromide (CrSBr) using a cryogenic near-infrared near-field microscope. At low temperatures, in the magnetically-ordered state, anisotropic exciton resonances sharpen, driving the permittivity negative along one crystal axis and enabling HEP propagation. We characterize HEP momentum and losses in CrSBr, also demonstrating coupling to excitonic sidebands and enhancement by magnetic order: which boosts exciton spectral weight via wavefunction delocalization. Our findings open new pathways to nanoscale manipulation of excitons and light, including routes to magnetic, nonlocal, and quantum polaritonics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Sensitivity of the MnTe valence band to the orientation of magnetic moments

An effective model of the hexagonal (NiAs-structure) manganese telluride valence band in the vicinity of the A point of the Brillouin zone is derived. It is shown that whereas for the usual antiferromagnetic order (magnetic moments on the basal plane) band splitting at A is small, their out-of-plane rotation enhances the splitting dramatically (to about 0.5 eV). Here we propose extensions of recent experiments where such inversion of magnetocrystalline anisotropy has been observed in Li-doped MnTe to confirm this unusual sensitivity of a semiconductor band structure to magnetic order.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Pressure-tuning of the electronic and magnetic properties of EuPt 2 Si 2

Using the element and orbital selectivity of x-ray absorption spectroscopy at Eu and Pt L 3 edges we investigate the effects of the lattice contraction, induced by temperature and external pressure, on the magnetic and electronic properties of the EuPt 2 Si 2 system. Our findings point to a clear relationship between the volume and the Eu valence in this material. From XANES experiments as a function of pressure we show that the Europium valence tends to stabilize at 3+ for pressures up to 27 GPa. The XMCD results demonstrate that pressure induced valence change of the Europium ion leads to a suppression of the magnetic ordering of the material. Finally, altogether our results provide direct evidence that Eu-4f /5d electronic hybridization effects underlie the mechanism that regulates the valence and magnetic ordering in this material.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Gapless dispersive continuum in a modulated quantum kagome antiferromagnet

The pursuit of quantum spin liquid (QSL) states in condensed matter physics has drawn attention to kagome antiferromagnets (AFM) where a two-dimensional corner-sharing network of triangles frustrates conventional magnetic orders. While quantum kagome AFMs based on Cu 2+ (3d 9 , s = 1/2) ions have been extensively studied, there is so far little work beyond copper-based systems. Here we present our bulk magnetization, specific heat and neutron scattering studies on single crystals of a new titanium fluorides Cs 8 RbK 3 Ti 12 F 48 where Ti 3+ (3d 1 , s = 1/2) ions form a modulated quantum kagome antiferromagnet that does not order magnetically down to 1.5 K. Our comprehensive map of the dynamic response function $S$($Q$,$\hslash$$\omega$) acquired at 1.5 K where the heat capacity is T-linear reveals a dispersive continuum emanating from soft lines that extend along (100). The data indicate fractionalized spinon-like excitations with quasi-one-dimensional dispersion within a quasi-two-dimensional spin system.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗