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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 181 records · Page 10
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Spin-coupling topology in the copper hexamer compounds A 2 Cu 3 O(SO 4 ) 3 ( A =Na, K)

The compounds A 2 Cu 3 O(SO 4 ) 3 (A=Na,K) are characterized by copper hexamers that are weakly coupled to realize antiferromagnetic order below TN≈3K. They constitute quantum spin systems with S=1 triplet ground states. In this work, we investigated the energy-level splittings of the copper hexamers by inelastic neutron scattering experiments covering the entire range of the magnetic excitation spectra. Additionally, the observed transitions are governed by very unusual selection rules that we ascribe to the underlying spin-coupling topology. This is rationalized by model calculations that allow an unambiguous interpretation of the magnetic excitations concerning both the peak assignments and the nature of the spin-coupling parameters.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Non-Altermagnetic Origin of Exchange Bias Behaviors in Incoherent RuO 2 /Fe Bilayer Heterostructures

Initially identified as a promising altermagnetic (AM) candidate, rutile RuO 2 has since become embroiled in controversy due to contradictory findings of modeling and measurements of the magnetic properties of bulk crystals and thin films. For example, despite observations of a bulk nonmagnetic state using density functional theory, neutron scattering, and muon spin resonance measurements, patterned RuO 2 Hall bars and film heterostructures display magnetotransport signatures of magnetic ordering. Among the characteristics routinely cited as evidence for AM is the observation of exchange bias (EB) in an intimately contacted Fe-based ferromagnetic (FM) layer, which can arise due to interfacial coupling with a compensated antiferromagnet. Here, within this work, the origins of this EB coupling in Ru-capped RuO 2 /Fe bilayers are investigated using polarized neutron diffraction, polarized neutron reflectometry, cross-sectional transmission electron microscopy, and super conducting quantum interference device measurements. These experiments reveal that the EB behavior is driven by the formation of an iron oxide interlayer containing Fe 3 O 4 that undergoes a magnetic transition and pins interfacial moments within Fe at low temperature. These findings are confirmed by comparable measurements of Ni-based heterostructures, which do not display EB coupling, as well as magnetometry of additional Fe/Ru bilayers that display oxide-driven EB coupling despite the absence of the epitaxial RuO 2 layer. While these results do not directly refute the possibility of AM ordering in RuO 2 thin films, they reveal that EB, and related magnetotransport phenomena, cannot alone be considered evidence of this characteristic in the rutile structure due to interfacial chemical disorder.

RuO2↗
DOE OSTI2021

Mirror symmetry breaking in a model insulating cuprate

Among the most actively studied issues in the cuprates are the natures of the pseudogap and strange metal states and their relationship to superconductivity. There is general agreement that the low-energy physics of the Mott-insulating parent state is well captured by a two-dimensional spin S = 1/2 antiferromagnetic Heisenberg model. However, recent observations of a large thermal Hall conductivity in several parent cuprates appear to defy this simple model and suggest proximity to a magneto-chiral state that breaks all mirror planes that are perpendicular to the CuO 2 layers. Here we use optical second harmonic generation to directly resolve the point group symmetries of the model parent cuprate Sr 2 CuO 2 Cl 2 . We report evidence of an order parameter that breaks all perpendicular mirror planes and is consistent with a magneto-chiral state in zero magnetic field. Although this order is clearly coupled to the antiferromagnetism, we are unable to realize its time-reversed partner by thermal cycling through the antiferromagnetic transition temperature or by sampling different spatial locations. Finally, this suggests that the order onsets above the Neel temperature and may be relevant to the mechanism of pseudogap formation.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2020

Detection of uncompensated magnetization at the interface of an epitaxial antiferromagnetic insulator

We have probed directly the temperature and magnetic field dependence of pinned uncompensated magnetization at the interface of antiferromagnetic FeF 2 with Cu, using FeF 2 -Cu-Co spin valves. Electrons polarized by the Co layer are scattered by the pinned uncompensated moments at the FeF 2 -Cu interface giving rise to giant magnetoresistance. We determined the direction and magnitude of the pinned uncompensated magnetization at different magnetic fields and temperatures using the angular dependencies of resistance. The strong FeF 2 anisotropy pins the uncompensated magnetization along the easy axis independent of the cooling field orientation. Most interestingly, magnetic fields as high as 90 kOe cannot break the pinning at the FeF 2 -Cu interface. This proves that the pinned interfacial magnetization is strongly coupled to the antiferromagnetic order inside the bulk FeF 2 layer. Studies as a function of FeF2 crystalline orientation show that uncompensated spins are only detected in a spin valve with (110) crystal orientation, but not in valves containing FeF 2 (100) and FeF 2 (001). This observation is in agreement with symmetry-related considerations which predict the equilibrium boundary magnetization for the FeF 2 (110) layer.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Terahertz stimulated parametric downconversion of a magnon mode in an antiferromagnet

Parametric amplification, where one signal is enhanced by the action of another, offers both practical utility for boosting weak signals and fundamental insights into the nonlinear coupling between degrees of freedom. In condensed matter systems, interactions between collective modes offer avenues for nonlinear coherent manipulation of coupled excitations and quantum phases. Antiferromagnets, with inherently coupled magnon modes, provide a promising platform for nonlinear control of spin waves and magnetization. However, nonlinear magnon-magnon interactions have been only partially elaborated, leaving key gaps in the prospects for potential ultrahigh-bandwidth magnonic signal processing. Here, we excite two distinct coherent magnon modes in an antiferromagnet and find that the magnon mode with a lower frequency undergoes amplification when the higher-frequency mode is driven. We unveil the nonlinear excitation pathways of this stimulated parametric downconversion process by using polarization-selective two-dimensional terahertz spectroscopy. Our work provides fundamental insights into nonlinear magnonics in antiferromagnets, laying the groundwork for forthcoming spintronic and magnonic devices.

Science & Technology - Other Topics↗
DOE OSTI2021

Stripe antiferromagnetic ground state of the ideal triangular lattice compound KErSe 2

Rare-earth triangular lattice materials have been proposed as a good platform for the investigation of frustrated magnetic ground states. KErSe 2 , with the delafossite structure, contains perfect two-dimensional Er 3 + triangular layers separated by potassium ions, realizing this ideal configuration and inviting study. In this study, we investigate the magnetism of KErSe 2 at millikelvin temperatures by heat capacity and neutron powder diffraction. Heat capacity results reveal a magnetic transition at 0.2 K in zero applied field. This long-range order is suppressed by an applied magnetic field of 0.5 T below 0.08 K. Neutron powder diffraction suggests that the zero-field magnetic structure orders with k = ( 1 2 , 0 , 1 2 ) in a stripe spin structure. Unexpectedly, Er is found to have a reduced moment of 3.06(1) μ B /Er in the ordered state, and diffuse magnetic scattering, which originates at higher temperatures, is found to persist in the ordered state, potentially indicating magnetic fluctuations. Neutron diffraction collected under an applied field shows a metamagnetic transition at ~ 0.5 T to ferromagnetic order with k = ( 0 , 0 , 0 ) and two possible structures, which are likely dependent on the applied field direction. The zero-field stripe spin structure can be explained by the anisotropic interactions or the first-, second-, and third-neighbor couplings in the antiferromagnetic triangular lattice.

2-dimensional systems↗
DOE OSTI2020

Insensitivity of Magnetic Coupling to Ligand Substitution in a Series of Tetraoxolene Radical-Bridged Fe 2 Complexes

The elucidation of magnetostructural correlations between bridging ligand substitution and strength of magnetic coupling is essential to the development of high-temperature molecule-based magnetic materials. Toward this end, we report the series of tetraoxolene-bridged Fe II 2 complexes [(Me 3 TPyA) 2 Fe 2 ( R L)] n + (Me 3 TPyA = tris(6-methyl-2-pyridylmethyl)amine; n = 2: OMe LH 2 = 3,6-dimethoxy-2,5-dihydroxo-1,4-benzoquinone, Cl LH 2 = 3,6-dichloro-2,5-dihydroxo-1,4-benzoquinone, Na 2 [ NO 2 L] = sodium 3,6-dinitro-2,5-dihydroxo-1,4-benzoquinone; n = 4: SMe 2 L = 3,6-bis(dimethylsulfonium)-2,5-dihydroxo-1,4-benzoquinone diylide) and their one-electron-reduced analogues. Furthermore, variable-temperature dc magnetic susceptibility data reveal the presence of weak ferromagnetic superexchange between Fe II centers in the oxidized species, with exchange constants of J = +1.2(2) (R = OMe, Cl) and +0.3(1) (R = NO 2 , SMe 2 ) cm –1 . In contrast, X-ray diffraction, cyclic voltammetry, and Mössbauer spectroscopy establish a ligand-centered radical in the reduced complexes. Magnetic measurements for the radical-bridged species reveal the presence of strong antiferromagnetic metal–radical coupling, with J = -57(10), -60(7), -58(6), and -65(8) cm –1 for R = OMe, Cl, NO 2 , and SMe 2 , respectively. The minimal effects of substituents in the 3- and 6-positions of R L x –• on the magnetic coupling strength is understood through electronic structure calculations, which show negligible spin density on the substituents and associated C atoms of the ring. Finally, the radical-bridged complexes are single-molecule magnets, with relaxation barriers of U eff = 50(1), 41(1), 38(1), and 33(1) cm –1 for R = OMe, Cl, NO 2 , and SMe 2 , respectively. Taken together, these results provide the first examination of how bridging ligand substitution influences magnetic coupling in semiquinoid-bridged compounds, and they establish design criteria for the synthesis of semiquinoid-based molecules and materials.

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

Physical properties of intergrowth compound Eu 2 CuZn 2 P 3

Here, the physical properties of single-crystalline Eu 2 ⁢CuZn 2 ⁢P 3 were inspected via thermodynamic, transport, and neutron diffraction measurements. Eu 2 ⁢ CuZn 2⁢ P 3 is composed of EuCuP and EuZn 2 ⁢ P 2 motifs stacked in a one-to-one ratio. The magnetic response of Eu 2 ⁢ CuZn 2 ⁢ P 3 is similar to that of EuZn 2 ⁢ P 2 in its A-type antiferromagnetic (semiconducting) state. A Néel temperature of T N = 40.3K is obtained from the specific heat capacity. Single-crystal neutron diffraction reveals a (001) magnetic propagation vector, with primarily in-plane moments coupled along [001] in an up-up-down-down pattern. This spin structure retains the ferromagnetic EuCuP motifs and antiferromagnetic coupling across the EuZn 2 ⁢P 2 motifs. The electrical resistivity is characterized by metallic behavior above 100 K, an increase in ρ upon cooling below ≈ 75K, and a large negative magnetoresistance below T N . First principles calculations evidence a narrow band gap for antiferromagnetic ordering and semimetallic behavior for the ferromagnetic state. This is consistent with the observed effect of magnetic field on the electrical resistivity. Hall effect measurements reveal a field-induced, negative anomalous Hall effect that increases on cooling down to 2 K. Also, an unconventional contribution to the Hall effect dominates the low-field Hall signal, particularly near T N , and is similar in appearance to a topological Hall effect. However, further work is necessary to understand if any of the transport properties have topological origins or if magnetism-induced modifications to the Fermi surface induce these unusual Hall effect signals in this and related materials.

36 MATERIALS SCIENCE↗
DOE OSTI2024

ASb 3 Mn 9 O 19 (A = K or Rb): New Mn-Based 2D Magnetoplumbites with Geometric and Magnetic Frustration

Magnetoplumbites are one of the most broadly studied families of hexagonal ferrites, typically with high magnetic ordering temperatures, making them excellent candidates for permanent magnets. However, magnetic frustration is rarely observed in magnetoplumbites. Herein, the discovery, synthesis, and characterization of the first Mn-based magnetoplumbite, as well as the first magnetoplumbite involving pnictogens (Sb), ASb 3 Mn 9 O 19 (A = K or Rb) are reported. The Mn 3+ ( S = 2) cations, further confirmed by DC magnetic susceptibility and X-ray photoelectron spectroscopy, construct three geometrically frustrated sublattices, including Kagome, triangular, and puckered honeycomb lattices. Magnetic properties measurements revealed strong antiferromagnetic spin–spin coupling as well as multiple low-temperature magnetic features. Heat capacity data does not show any prominent λ-anomaly, suggesting minimal associated magnetic entropy. Moreover, neutron powder diffraction (NPD) implied the absence of long-range magnetic ordering in KSb 3 Mn 9 O 19 down to 3 K. However, several magnetic peaks are observed in RbSb 3 Mn 9 O 19 at 3 K, corresponding to an incommensurate magnetic structure. Interestingly, strong diffuse scattering is seen in the NPD patterns of both compounds at low angles and is analyzed by reverse Monte Carlo refinements, indicating short-range spin ordering related to frustrated magnetism as well as 2D magnetic correlations in ASb 3 Mn 9 O 19 (A = K or Rb).

2-D magnetic correlation↗
DOE OSTI2021

Structure, Magnetism, and First-Principles Modeling of the Na 0.5 La 0.5 RuO 3 Perovskite

High-purity polycrystalline Na 0.5 La 0.5 RuO 3 was synthesized by a solid-state method, and its properties were studied by magnetic susceptibility, heat capacity, and resistivity measurements. In this study, we find it to be an orthorhombic perovskite, in contrast to an earlier report, with random La/Na mixing. With a Curie–Weiss temperature of –231 K and an effective moment of 2.74 μB/mol Ru, there is no magnetic ordering down to 1.8 K. A broad hump at 1.4 K in the heat capacity, however, indicates the presence of a glassy magnetic transition, which we attribute to the influence of the random distribution of Na and La on the perovskite A-sites. Comparison to CaRuO 3 , a structurally ordered ruthenate perovskite with a similar A-site ionic radius and magnetic properties, is presented. First-principles calculations indicate that the Na–La distribution determines the local magnetic exchange interactions between Ru ions, favoring either antiferromagnetic or ferromagnetic coupling when the local environment is Na- or La-rich. Thus, our data and analysis suggest that mixing cations with different charges and sizes on the A-site in this perovskite results in magnetic frustration through a balance of local magnetic exchange interactions.

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

Anyon superconductivity from topological criticality in a Hofstadter–Hubbard model

We argue that the combination of strong repulsive interactions and high magnetic fields can generate electron pairing and superconductivity. Inspired by the large lattice constants of moiré materials, which make large flux per unit cell accessible at laboratory fields, we study the triangular lattice Hofstadter-Hubbard model at one-quarter flux quantum per plaquette, where previous literature has argued that a chiral spin liquid separates a weak-coupling integer quantum Hall phase and a strong-coupling topologically trivial antiferromagnetic insulator at a density of one electron per site. We argue that topological superconductivity emerges upon doping in the vicinity of the integer quantum Hall to chiral spin liquid transition. We employ exact diagonalization and density matrix renormalization group methods to examine this theoretical scenario and find that electronic pairing indeed occurs on both sides of criticality over a remarkably broad range of interaction strengths. On the chiral spin liquid side, our results provide a concrete model realization of the long-hypothesized mechanism of anyon superconductivity. Our study thus establishes a beyond-Bardeen-Cooper-Schrieffer route to electron pairing in a well-controlled limit, relying crucially on the interplay between electron correlations and band topology.

Hubbard model↗
DOE OSTI2022

Slow spin dynamics in the hyperhoneycomb lattice [ ( C 2 H 5 ) 3 NH ] 2 Cu 2 ( C 2 O 4 ) 3 revealed by H 1 NMR studies

We report the results of magnetic susceptibility χ and H 1 nuclear magnetic resonance (NMR) measurements on a three-dimensional hyperhoneycomb lattice compound [ ( C 2 H 5 ) 3 NH ] 2 Cu 2 ( C 2 O 4 ) 3 (CCCO). The average value of the antiferromagnetic (AFM) exchange coupling between the Cu 2 + ( S = 1 / 2 ) spins was determined to be J ~ 50 K from the χ measurements. No long-range magnetic ordering has been observed down to T = 50 mK, although NMR lines become slightly broader at low temperatures below 1 K. The broadening of the NMR spectrum observed below 1 K reveals that the Cu spin moments remain at this temperature, suggesting a non-spin-singlet ground state. The temperature and magnetic field dependence of 1 / T 1 at temperatures above 20 K is well explained by paramagnetic thermal spin fluctuations where the fluctuation frequency of Cu 2 + spins is higher than the NMR frequency of the order of megahertz. However, a clear signature of the slowing down of the Cu 2 + spin fluctuations was observed at low temperatures where 1 / T 1 shows a thermally activated behavior. The magnetic field dependence of the magnitude of the spin excitation gap suggests that the magnetic behaviors of CCCO are characterized as an AFM chain at low temperatures.

1-dimensional systems↗
DOE OSTI2024

Effects of pressure on the electronic and magnetic properties of bulk NiI 2

Transition metal dihalides have recently garnered interest in the context of two-dimensional van der Waals magnets as their underlying geometrically frustrated triangular lattice leads to interesting competing exchange interactions. In particular, NiI 2 is a magnetic semiconductor that has been long known for its exotic helimagnetism in the bulk. Recent experiments have shown that the helimagnetic state survives down to the monolayer limit with a layer-dependent magnetic transition temperature that suggests a relevant role of the interlayer coupling. Here, we explore the effects of hydrostatic pressure as a means to enhance this interlayer exchange and ultimately tune the electronic and magnetic response of NiI 2 . We study first the evolution of the structural parameters as a function of external pressure using first-principles calculations combined with x-ray diffraction measurements. We then examine the evolution of the electronic structure and magnetic exchange interactions via first-principles calculations and Monte Carlo simulations. Further, we find that the leading interlayer coupling is an antiferromagnetic second-nearest-neighbor interaction that increases monotonically with pressure. The ratio between isotropic third- and first-nearest-neighbor intralayer exchanges, which controls the magnetic frustration and determines the magnetic propagation vector q of the helimagnetic ground state, is also enhanced by pressure. As a consequence, our Monte Carlo simulations show a monotonic increase in the magnetic transition temperature, indicating that pressure is an effective means to tune the magnetic response of NiI 2 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Soliton formation and topology manipulation of coupled spins via ultrafast re-magnetization

The major goal of the project was to explore the properties of magnetic order driven far out of equilibrium by optical excitations. These include fundamental questions related to the interplay of magnetic, structural and electronic degrees of freedom in materials that are optically excited. These problems break down in short term quenching of the magnetization as a results of the energy of the optical pulse studying how the energy of the optical pulse and the angular momentum of the magnetization flow between the different degrees of freedom. This is followed by the longer time re-emergence of the magnetism as the system cools. Within this goal we explored the formation of solitons, both with and without non-trivial topology, via rapid re-magnetization processes after optical-driven ultrafast demagnetization. Guided by theory, we predict that turbulence and modulational instabilities will drive the formation of solitons, including dispersive shock waves, magnon droplets, and skyrmions. In the case of topological defect formation, i.e. skyrmion generation, related processes have long been predicted based on general principles of symmetry-breaking phase transitions; the density of topological defects in a long-range-ordered phase can be controlled by varying the quench rate through the second-order phase transition, i.e. the Kibble-Zurek (KZ) mechanism. We, more broadly, had the goal to study a range of other emergent magnetic behaviors after optical excitation. While great attention has been given to ultrafast demagnetization, less is known of the subsequent spin dynamics and coupling to the lattice. What is increasingly appreciated is that ultrafast demagnetization leads to spin currents that can carry angular momentum from the rapidly demagnetized sample. These spin currents appear in many ways but fundamentally controls demagnetization, drives interactions between regions of the material, and control the spin resulting structure. They can be probed many ways including THz emission which, in turn, gives insight into the demagnetization processes. Simultaneously if there is magneto-elastic coupling ultrafast demagnetization can drive structural excitations that are not expected from thermal energy added to the lattice. We explored a range of complex phenomena that arise from photo-excitation of magnetic systems with the coupling of electronic, magnetic and structural degrees of freedom. We have made a number of fundamental discoveries that are reflected in our publications list with additional work still being prepared for publication. Highlights of this work include (i) ultra-efficient, nonlinear THz surface acoustics (ii) spin-current-mediated rapid magnon localization and coalescence, (iii) spin-wave soliton formation in ferromagnetic FePt nanoparticles, (iv) dynamic phonon coupling in elemental antiferromagnetic Cr, (v) THz emission from Co/Pt bilayers and FeRh/Pt bilayers, (vi) theoretical investigation of spin hydrodynamics, solitons and shock waves, and (vii) ultrafast perturbation of magnetic domains by optical pumping.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Dirac-fermion-assisted interfacial superconductivity in epitaxial topological-insulator/iron-chalcogenide heterostructures

Abstract Over the last decade, the possibility of realizing topological superconductivity (TSC) has generated much excitement. TSC can be created in electronic systems where the topological and superconducting orders coexist, motivating the continued exploration of candidate material platforms to this end. Here, we use molecular beam epitaxy (MBE) to synthesize heterostructures that host emergent interfacial superconductivity when a non-superconducting antiferromagnet (FeTe) is interfaced with a topological insulator (TI) (Bi, Sb) 2 Te 3 . By performing in-vacuo angle-resolved photoemission spectroscopy (ARPES) and ex-situ electrical transport measurements, we find that the superconducting transition temperature and the upper critical magnetic field are suppressed when the chemical potential approaches the Dirac point. We provide evidence to show that the observed interfacial superconductivity and its chemical potential dependence is the result of the competition between the Ruderman-Kittel-Kasuya-Yosida-type ferromagnetic coupling mediated by Dirac surface states and antiferromagnetic exchange couplings that generate the bicollinear antiferromagnetic order in the FeTe layer.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Spin-Charge-Lattice Coupling across the Charge Density Wave Transition in a Kagome Lattice Antiferromagnet

Understanding spin and lattice excitations in a metallic magnetic ordered system forms the basis to unveil the magnetic and lattice exchange couplings and their interactions with itinerant electrons. Kagome lattice antiferromagnet FeGe is interesting because it displays a rare charge density wave (CDW) deep inside the antiferromagnetic ordered phase that interacts with the magnetic order. Here, we use neutron scattering to study the evolution of spin and lattice excitations across the CDW transition 𝑇 CDW in FeGe. While spin excitations below ∼100 meV can be well described by spin waves of a spin-1 Heisenberg Hamiltonian, spin excitations at higher energies are centered around the Brillouin zone boundary and extend up to ∼180 meV consistent with quasiparticle excitations across spin-polarized electron-hole Fermi surfaces. Furthermore, 𝑐-axis spin wave dispersion and Fe-Ge optical phonon modes show a clear hardening below 𝑇 CDW due to spin-charge-lattice coupling but with no evidence of a phonon Kohn anomaly. By comparing our experimental results with density functional theory calculations in absolute units, we conclude that FeGe is a Hund’s metal in the intermediate correlated regime where magnetism has contributions from both itinerant and localized electrons arising from spin polarized electronic bands near the Fermi level.

charge density waves↗
DOE OSTI2025

Atomic dynamics in 𝑀⁢Cr⁢𝑋 2 (𝑀=Ag, Cu; 𝑋 = S, Se) across magnetic and superionic transitions

Here, a systematic study of atomic dynamics and thermal properties of the family of layered chalcogenide compounds 𝑀⁢Cr⁢𝑋 2 (𝑀= Ag, Cu; 𝑋 = S, Se) was performed, including neutron and x-ray scattering, thermal characterization, and first-principles simulations. In all compounds, we observe a breakdown of specific phonon modes across the superionic phase transition, for phonons whose eigenvectors exhibit large contributions of mobile ions. In particular, the nondispersive portions of transverse acoustic (TA) branches at short-wavelengths and the low-energy optical phonons with large contributions from Ag + or Cu + become severely damped in the superionic phase. However, well-defined quasiparticles persist in the superionic state for long-wavelength TA phonons. In the case of AgCrS 2 , the coupling of lattice dynamics with its antiferromagnetic transition was also investigated. The magnetic ordering couples with the monoclinic–rhombohedral structural transition, and the Cr 3+ spin arrangement strongly affects the phonon dispersions. We qualitatively reproduce the magnetic and nuclear components of the INS measurement for antiferromagnetic AgCrS 2 by combining models of spin-waves and spin-polarized first-principles phonon simulations. Quasielastic magnetic fluctuations persist in the paramagnetic phase up to high temperature, but are clearly distinguished from the nuclear component through their momentum dependence. Finally, we report measurements of the thermal properties of the selenide compounds and find good agreement with our DFT simulations.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Magnetic and quadrupole coupling emerging in NdB 4 with geometrically frustrated orthogonal antiferromagnetic dimer

Unusual successive order in NdB 4 with the frustrated Shastry-Sutherland lattice was investigated by means of inelastic neutron scattering. Here, we found that the pseudoquartet with |±5/2⟩ and |±7/2⟩ in the paramagnetic state splits into four levels in the magnetically ordered states. The observed spectra are in good agreement with the 𝑓-electron states obtained from the on-site Hamiltonian with the magnetic interaction ⟨𝐽 𝑥 ⟩ ⁢𝐽 𝑥 , the coupling of 𝐽 𝑥 with quadrupole 𝑂 𝑧⁢𝑥 , and the crystalline electric field potential. The 𝑓-electron states reproduce the temperature dependences of the in-plane moment 𝑚 ⊥ = ⟨𝐽 𝑥 ⟩, which is the primary order parameter, and a weakly induced 𝑚 𝑐 = ⟨𝐽 𝑧 ⟩ as the secondary order parameter. The magnetic-quadrupole coupling emerges and plays an essential role under the geometrical frustration, where the Heisenberg interactions are canceled out.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗