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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Quantum Effect on the Ground State of the Triple-Perovskite Ba 3 MNb 2 O 9 (M = Co, Ni, and Mn) with Triangular-Lattice

As the simplest example of geometrical frustration, the two-dimensional triangular lattice antiferromagnet exhibits the mismatch between the lattice geometry and spin-exchange interaction, which has been the subject of intensive studies due to its exotic quantum phenomena. In this work, we performed detailed studies of the magnetic structures and spin wave excitations by neutron powder diffraction and inelastic neutron scattering measurements on the triple-perovskite oxides Ba 3 MNb 2 O 9 (M = Co, Ni, and Mn) with triangular-lattice geometry. The interplay between the frustrated interaction and easy-plane/axis anisotropy gives rise to two magnetic phase transition temperatures for Ba 3 CoNb 2 O 9 (Ba 3 MnNb 2 O 9 ) and only one for Ba 3 NiNb 2 O 9 . The linear spin-wave theory +1/S calculations indicate that both spatial dimensionality and the spin size have a significant impact on the strength of quantum fluctuations, which lead to their different magnetic ground states and exotic physical properties. Moreover, the effects of the thermal fluctuations are presented for Ba 3 NiNb 2 O 9 .

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

Single crystal synthesis and magnetic properties of a Shastry-Sutherland lattice compound BaNd 2 ZnS 5

In this study, single crystals of a Shastry-Sutherland magnetic semiconductor, BaNd 2 ZnS 5 , were synthesized through a high-temperature solution growth technique. Physical properties were characterized by powder and single crystal x-ray diffraction, temperature- and field-dependent magnetization, and temperature-dependent specific heat measurements. BaNd 2 ZnS 5 orders antiferromagnetically at 2.9 K, with magnetic moments primarily aligned within the $ab$ -plane. Magnetic isothermal measurements show metamagnetic transitions at ~ 15 kOe for the [110] direction and ~ 21 kOe for the [100] direction. Estimated magnetic entropy suggests a double ground state for each neodymium ion.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Cluster-Spin-Glass Magnetic Behavior and Morphology in the Coordination Polymer Alloys Fe y Co 1– y BTT

We report the synthesis of a series of pseudo-1D coordination polymer (CP) materials with the formula Fe y Co 1–y BTT (BTT = 1,3,5-benzenetrithiolate). These materials were structurally characterized by PXRD Rietveld, EXAFS, and PDF analyses, revealing that the CP superstructure enables a continuous and isomorphous alloy between the two homometallic compounds. Lower Fe loadings exhibit emergent spin glass magnetic behavior, such as memory effects and composition-dependent spin glass response time constants ranging from 6.9 × 10 –9 s to 1.8 × 10 –6 s. These data are consistent with the formation of spin clusters within the lattice. The magnetic behavior in these materials was modeled via replica exchange Monte Carlo simulation, which provides a good match for the experimentally measured spin glassing and magnetic phase transitions. Furthermore, these findings underscore how the rigid superstructure of CP and MOF scaffolds can enable the systematic tuning of physical properties, such as the spin glass behavior described here.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Low-field magnetic anomalies in single crystals of the A-type square-lattice antiferromagnet EuGa 4

The body-centered-tetragonal antiferromagnet EuGa 4 was recently identified as a Weyl nodal-line semimetal that exhibits the topological Hall effect below its reported antiferromagnetic (AFM) ordering temperature T N = 15 – 16.5 K which we find to be T N = 16.4 ( 2 ) K. The Eu +2 ions are located at the corners and body centers of the unit cells. EuGa 4 exhibits A-type antiferromagnetic order below T N , where the Eu 2+ spin-7/2 moments are ferromagnetically aligned in the ab plane with the Eu moments in adjacent Eu planes along the c axis aligned antiferromagnetically. Low-field magnetization versus field M(H ab ) data at T = 2 K with the field aligned in the ab plane are reported that exhibit anomalous positive curvature up to a critical field H c1 at which a second-order transition occurs with H c1 ≈ 0.85 kOe for H∥ [1,1,0] and ≈ 4.8 kOe for H∥[1,0,0]. For larger fields, the linear behavior M ab = χ(T N ) H a b is followed until the critical field H c is reached at which all moments become aligned with the applied field. A theory is formulated for T = 0 K that fits the observed M(H ab ) behavior at T = 2 K well, where domains of A -type AFM order with fourfold rotational symmetry occur in the AFM state in zero field. The moments in the four domains reorient to become almost perpendicular to H ab at H c1 , followed by increasing canting of all moments toward the field with increasing field up to H c which is reported to be 71 kOe. A first-order transition in M(H ab ) at H ab = H c1 is predicted by the theory for T = 0 K when H ab is at a small angle from the [1,0,0] direction.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Nontrivial critical behavior at magnetic transitions: A case study of Sm 7 ⁢Pd 3

We present a comprehensive analysis of the critical behavior of Sm 7 ⁢Pd 3 in the vicinity of its second-order magnetoelastic transition at 𝑇 c =173 K. The critical exponents (CEs) 𝛽 and 𝛾, determined using both the standard convergence procedure and the average normalized slope (ANS) method, diverge at 𝑇 c –-a characteristic typically associated with first-order transitions. Notably, none of the established universality classes satisfactorily describe the critical behavior of Sm 7 ⁢Pd 3 , and we discuss the possible origins of this deviation in the context of the strong spin-lattice coupling intrinsic to the sample. We emphasize the importance of accurately selecting the critical temperature and magnetic field ranges to ensure robust critical behavior analysis, and propose a quantitative approach to assess the reliability of the extracted CEs. Additionally, we demonstrate that in the ANS method, the critical exponents 𝛽 and 𝛾 should be calculated separately using data for 𝑇 ⩽ 𝑇 c and 𝑇 ⩾ 𝑇 c , respectively. In conclusion, our findings underscore the need for a revised theoretical framework to accurately describe second-order magnetoelastic transitions.

Ferrimagnets↗
DOE OSTI2024

Colossal magnetoresistance from spin-polarized polarons in an Ising system

Recent experiments suggest a new paradigm toward novel colossal magnetoresistance (CMR) in a family of materials EuM 2 X 2 (M = Cd, In, Zn; X = P, As), distinct from the traditional avenues involving Kondo–Ruderman–Kittel–Kasuya–Yosida crossovers, magnetic phase transitions with structural distortions, or topological phase transitions. Here, we use angle-resolved photoemission spectroscopy and density functional theory calculations to explore their origin, particularly focusing on EuCd 2 P 2 . While the low-energy spectral weight royally tracks that of the resistivity anomaly near the temperature with maximum magnetoresistance ( T MR ) as expected from transport-spectroscopy correspondence, the spectra are completely incoherent and strongly suppressed with no hint of a Landau quasiparticle. Using systematic material and temperature dependence investigation complemented by theory, we attribute this nonquasiparticle caricature to the strong presence of entangled magnetic and lattice interactions, a characteristic enabled by the p - f mixing. Given the known presence of ferromagnetic clusters, this naturally points to the origin of CMR being the scattering of spin-polarized polarons at the boundaries of ferromagnetic clusters. These results are not only illuminating to investigate the strong correlations and topology in EuCd 2 X 2 family, but, in a broader view, exemplify how multiple cooperative interactions can give rise to extraordinary behaviors in condensed matter systems.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Anisotropic magnetocaloric effect and critical behavior in CrCl 3

We report anisotropic magnetocaloric effect and magnetic critical behavior in the van der Waals crystal CrCl 3 . The maximum magnetic entropy change $-ΔS^{max}_M ~ 14.6 J kg -1 K -1 and the relative cooling power RCP ~ 340.3 J kg -1 near T c with a magnetic field change of 5 T are much larger when compared to CrI 3 or CrBr 3 . The rescaled ΔS M (T, H) curves collapse onto a universal curve, confirming the second-order ferromagnetic transition. Finally, further critical behavior analysis around T c presents a set of critical exponents β = 0.28 (1) with T c = 19.4 (2) K, γ = 0.89 (1) with T c = 18.95 (8) K, and δ = 4.6 (1) at T c = 19 K , which are close to those of the theoretical tricritical mean-field model.

2-dimensional systems↗
DOE OSTI2022

Incommensurate spin density wave and magnetocaloric effect in the metallic triangular lattice HoAl 2 Ge 2

Here, we report the magnetic structure and the magnetocaloric effect (MCE) of the ternary compound HoAl 2 Ge 2 with a trigonal CaAl 2 Si 2 -type crystal structure. A neutron powder diffraction experiment reveals that HoAl 2 Ge 2 exhibits an incommensurate spin density wave (SDW) with a propagation vector k=(0.23,0,0.06). The special arrangement of magnetic moments in HoAl 2 Ge 2 induces interesting physical phenomena and large magnetocaloric effects. The rise in resistivity at low temperatures indicates the effect of the SDW state in the electronic transport. The maximum magnetic-entropy change is –16.1J/kg K under a magnetic field change of 0–70 kOe for an isotropic HoAl 2 Ge 2 powder and it increases to –17.9J/kg K for a single crystal when the magnetic field (H) is applied parallel to the ab plane. A large rotating magnetic-entropy change of –5.1J/kg K for H=20 kOe in a HoAl 2 Ge 2 single crystal is obtained, which is closely associated to the magnetic anisotropy of the SDW order and its response to the external magnetic field. We discuss the large MCE in terms of the field-induced metamagnetic transition from the incommensurate SDW order to the ferromagnetic order. Our study establishes the triangular lattice R Al 2 Ge 2 (R=rare-earth elements) as a unique family of compounds to explore the existence of the incommensurate spin density waves and the correlated physical properties.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Tuning the magnetic properties of the CrMnFeCoNi Cantor alloy

Magnetic properties of more than 20 Cantor alloy samples of varying composition were investigated over a temperature range of 5 K to 300 K and in fields of up to 70 kOe using magnetometry and muon spin relaxation. Two transitions are identified: a spin-glass-like transition that appears between 55K and 190K, depending on composition, and a ferrimagnetic transition that occurs at approximately 43K in multiple samples with widely varying compositions. The magnetic signatures at 43K are remarkably insensitive to chemical composition. A modified Curie-Weiss model was used to fit the susceptibility data and to extract the net effective magnetic moment for each sample. The resulting values for the net effective moment were either diminished with increasing Cr or Mn concentrations or enhanced with decreasing Fe, Co, or Ni concentrations. Beyond a sufficiently large effective moment, the magnetic ground state transitions from ferrimagnetism to ferromagnetism. The effective magnetic moments, together with the corresponding compositions, are used in a global linear regression analysis to extract element-specific effective magnetic moments, which are compared to the values obtained by ab initio based density functional theory calculations. Finally, these moments provide the information necessary to controllably tune the magnetic properties of Cantor alloy variants.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Pressure control of the spin reorientation transition in the rare-earth orthoferrite YbFeO 3

YbFeO 3 is exceptional among the rare-earth orthoferrites for having the lowest spin-reorientation transition (SRT) temperature, T SRT ≃8K, which makes it particularly appealing to examine the interplay between noncollinear magnetism of the Fe sublattice and quasi-one-dimensional XXZ effective S = 1/2 chains of Yb 3+ moments. Our paper focuses on the magnetic dynamics of YbFeO 3 using inelastic neutron scattering (INS), at temperatures below and above the SRT, under an applied hydrostatic pressure of 2 GPa, and in magnetic fields up to 4 T. The low-energy zero-field excitation spectrum at ambient pressure and temperatures below the SRT is dominated by a gapped magnon mode of the Yb subsystem at 0.84 meV with a dispersion only in the [00L] direction. Above T SRT , a continuum appears on top of the magnon mode because of temperature population of the magnon band, and the gap decreases to around 0.4 meV. The INS spectra in the magnetic field, both above and below T SRT , are characterized by two well-separated gapped modes. The SRT is clearly visible at low fields B < 1T, but it gradually disappears at higher magnetic fields. The hydrostatic pressure of p = 2GPa effectively reduces the transition width, ΔT SRT , and keeps the SRT at higher fields up to B≃3T. Here, we discuss the effect of the applied pressure in the frame of the modified mean-field theory and show that in the vicinity of the T SRT the pressure tunes the fourth-order anisotropy constant that effectively reduces the ΔT SRT .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Probing putative orbital differentiation effects via Eu 2+ spin dynamics in Sr 1-x Eu x Fe 2 As 2

Here, in this work, we report x-ray powder diffraction, elemental analysis, electrical resistivity, magnetic susceptibility, specific heat, and electron spin resonance (ESR) in single crystals of Sr 1-x Eu x Fe 2 As 2 . We observed a breakdown of the previously reported scaling between the Eu 2+ Korringa relaxation rate obtained from ESR and the spin density wave temperature evolution for Sr-rich samples. This result suggests a distinct evolution of the orbital differentiation of the Fe 3d bands along the Sr-based series when compared to the Ba counterpart. We argue that this difference is related to a larger splitting between the structural (tetragonal-to-orthorhombic) and the Fe-driven spin density wave transitions induced by Eu doping in this series. In fact, our results indicate that the two transitions follow an opposite x-Eu dependence for Sr-concentrated samples. Our work shows that Sr 1-x Eu x Fe 2 As 2 series and the comparison with their Ba-based counterparts are exciting platforms to be explored for understanding the interplay among orbital differentiation, magnetism, and structural distortions in the iron pnictides

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Crystal growth and magnetic structure of ternary silicide Eu Pd 3 Si 2

The hexagonal CaCu 5 –type structure (P6/mmm) is the prototype for more than 100 ternary borides, gallides, and silicides, with general stoichiometry of RTM 3 X 2 (R=lanthanide/alkaline earth; TM=transition metal; X=B, Ga, Si, Ge). Here we report the synthesis, crystal structure, and bulk magnetic properties of polycrystalline and single crystal samples of EuPd 3 Si 2 and its nonmagnetic analog SrPd 3 Si 2 . Both compounds crystallize in the orthorhombic space group symmetry Imma (no. 74, Z = 2, oI12) displaying pseudohexagonal symmetry. Ferromagnetic (FM) order of Eu 2+ at T C1 =78K and a spin-reorientation transition at T C2 =5K appear as distinctive features in bulk magnetization, specific heat, and resistivity/resistance measurements. Neutron powder diffraction measurements on EuPd 3 Si 2 confirm FM order of the Eu 2+ spins below T C1 , with the spins aligned along the a axis below T C2 . Electronic band structure calculations corroborate the crystal structure and the FM state for EuPd 3 Si 2 , with a Pd d–band polarization in the same direction as the Eu 4f polarization, enhancing the observed spin moment.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Cluster Frustration in the Breathing Pyrochlore Magnet LiGaCr 4 S 8

We present a comprehensive neutron scattering study of the breathing pyrochlore magnet LiGaCr 4 S 8 . We observe an unconventional magnetic excitation spectrum with a separation of high and low-energy spin dynamics in the correlated paramagnetic regime above a spin-freezing transition at 12(2) K. By fitting to magnetic diffuse-scattering data, we parameterize the spin Hamiltonian. We find that interactions are ferromagnetic within the large and small tetrahedra of the breathing pyrochlore lattice, but antiferromagnetic further-neighbor interactions are also essential to explain our data, in qualitative agreement with density-functional theory predictions [Ghosh et al., npj Quantum Mater. 4, 63 (2019)]. We explain the origin of geometrical frustration in LiGaCr 4 S 8 in terms of net antiferromagnetic coupling between emergent tetrahedral spin clusters that occupy a face-centered lattice. Furthermore, our results provide insight into the emergence of frustration in the presence of strong further-neighbor couplings, and a blueprint for the determination of magnetic interactions in classical spin liquids.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

Intrinsic ferromagnetism and restrictive thermodynamic stability in MA$_{2}$N$_{4}$ and Janus VSiGeN$_{4}$ monolayers

The seminal experimental discovery of the remarkably stable MoSi 2 N 4 monolayer has led to a handful of predicted magnetic two-dimensional (2D) materials in the MA 2 Z 4 family (M = transition metals, A = Si, Ge, and Z = N, P, As). These magnetic monolayers were predicted to be dynamically stable, but none of them has been synthesized to date. In this Research Letter, from first-principles thermodynamic stability analysis, we demonstrate that only the nitrides are thermodynamically stable and this occurs under N-rich conditions. Based on this finding, we propose two ferromagnetic, semiconducting Janus monolayers in the family: VSiGeN 4 and VSiSnN 4 . They are both dynamically and thermally stable, but only the former is thermodynamically stable. Intriguingly, Janus VSiGeN 4 and VSiSnN 4 monolayers show weak in-plane anisotropy compared with the VSi 2 N 4 monolayer. Furthermore, these two emerging Janus magnetic semiconductors offer opportunities for studying 2D magnetism and spin control for spintronics applications.

2-dimensional systems↗
DOE OSTI2020

Pseudospin versus magnetic dipole moment ordering in the isosceles triangular lattice material K 3 Er(VO 4 ) 2

Spin- 1 / 2 antiferromagnetic triangular lattice models are paradigms of geometrical frustration, revealing very different ground states and quantum effects depending on the nature of anisotropies in the model. Due to strong spin orbit coupling and crystal field effects, rare-earth ions can form pseudospin- 1 / 2 magnetic moments with anisotropic single-ion and exchange properties. Thus, rare-earth-based triangular lattices enable the exploration of this interplay between frustration and anisotropy. Here we study one such case, the rare-earth double vanadate glaserite material K 3 Er ( VO 4 ) 2 , which is a quasi-two-dimensional (2D) isosceles triangular antiferromagnet. Our specific heat and neutron powder diffraction data from K 3 Er ( VO 4 ) 2 reveal a transition to long range magnetic order at T N = 155 ± 5 mK which accounts for all R ln 2 entropy. Furthermore, we observe what appears to be a coexistence of three-dimensional (3D) and quasi-2D order below T N . The quasi-2D order leads to an anisotropic Warren-like peak profile for ( h k 0 ) reflections, while the 3D order is best-described by layers of antiferromagnetic b -aligned moments alternating with layers of zero moment. Our magnetic susceptibility data reveal that Er 3 + takes on a strong X Y single-ion anisotropy in K 3 Er ( VO 4 ) 2 , leading to vanishing moments when pseudospins are oriented along c . Thus, the magnetic structure, when considered from the pseudospin point of view could comprise of alternating layers of b -axis and c -axis aligned antiferromagnetism.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Dynamical exponent of a quantum critical itinerant ferromagnet: A Monte Carlo study

Here we consider the effect of the coupling between two-dimensional (2D) quantum rotors near an XY ferromagnetic quantum critical point and spins of itinerant fermions. We analyze how this coupling affects the dynamics of rotors and the self-energy of fermions. A common belief is that near a q = 0 ferromagnetic transition, fermions induce an Ω/q Landau damping of rotors (i.e., the dynamical critical exponent is z = 3) and Landau overdamped rotors give rise to non-Fermi liquid fermionic self-energy Σ∝ω 2/3 . This behavior has been confirmed in previous quantum Monte Carlo (QMC) studies. Here we show that for the XY case the behavior is different. We report the results of large-scale quantum Monte Carlo simulations, which show that at small frequencies z = 2 and Σ∝ω 1/2 . We argue that the new behavior is associated with the fact that a fermionic spin is by itself not a conserved quantity due to spin-spin coupling to rotors, and a combination of self-energy and vertex corrections replaces 1/q in the Landau damping by a constant. We discuss the implication of these results to experiments.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Structural, electronic, and magnetic properties of nearly ideal J eff = 1/2 iridium halides

Heavy transition metal magnets with J e f f = 1 2 electronic ground states have attracted recent interest due to their penchant for hosting new classes of quantum spin liquids and superconductors. Unfortunately, model systems with ideal J e f f = 1 2 states are scarce due to the importance of noncubic local distortions in most candidate materials. In this work, we identify a family of iridium halide systems [i.e., K 2 Ir Cl 6 , K 2 Ir Br 6 , ( NH 4 ) 2 Ir Cl 6 , and Na 2 Ir Cl 6 · 6 ( H 2 O ) ] with Ir 4 + electronic ground states exhibiting extremely small deviations from the ideal J e f f = 1 2 limit. We also find ordered magnetic ground states for the three anhydrous systems, with single-crystal neutron diffraction on K 2 Ir Br 6 revealing type-I antiferromagnetism. This spin configuration is consistent with expectations for significant Kitaev exchange in a face-centered-cubic magnet. This work establishes that incorporating isolated Ir X 6 octahedra in materials, where X is a halogen ion with a low electronegativity, is an effective design principle for realizing unprecedented proximity to the pure J e f f = 1 2 state. However, at the same time, we highlight undeniable deviations from this ideal state, even in clean materials with ideal Ir X 6 octahedra as inferred from the global cubic crystal structures.

36 MATERIALS SCIENCE↗
DOE OSTI2020

In-situ fabrication and transport properties of (111) Y 2 Ir 2 O 7 epitaxial thin film

We report on the successful fabrication of (111) oriented thin films of pyrochlore iridate Y 2 Ir 2 O 7 by means of solid phase epitaxy. Essentially, we developed an entirely in situ annealing protocol, which is superior to the conventional ex-situ routine that requires multi-hour annealing to stabilize the proper pyrochlore structure. The morphological quality of the films has been confirmed by x-ray diffraction, reflectivity, and reciprocal space mapping, demonstrating their high crystallinity with a pure pyrochlore phase and an expected epitaxial relation to the substrate. Strikingly, below the magnetic phase transition, the temperature dependence of resistivity shows a power-law behavior with the power exponent of similar to 3/2, characteristic of a Weyl semimetal in the presence of impurities and electron-electron correlations. Finally, below 10K, the magneto-transport measurements reveal the emergence of a non-saturated negative magnetoresistance up to 9T with a small "valley" around zero field. These findings are further interpreted in relation to the weak anti-localization effect and the non-collinear antiferromagnetic ordering on the Ir sublattice.

36 MATERIALS SCIENCE↗