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At least 1,063 records · Page 59
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Short-range order in the quantum XXZ honeycomb lattice material BaCo 2 ( PO 4 ) 2

In this paper, we present observations of highly frustrated quasi-two-dimensional (2D) magnetic correlations in the honeycomb lattice layers of the S eff =1/2 compound γ-BaCo 2 (PO 4 ) 2 (γ-BCPO). Specific heat shows a broad peak comprised of two weak kink features at T N1 ~6 K and T N2 ~3.5 K, the relative weights of which can be modified by sample annealing. Neutron powder diffraction measurements reveal short range quasi-2D order that is established below T N1 and T N2 , at which two separate, incompatible, short range magnetic orders onset: commensurate antiferromagnetic correlations with correlation length ξ c =60±2 Å (T N1 ) and in quasi-2D helical domains with ξ h =350±11 Å (T N2 ). The ac magnetic susceptibility response lacks frequency dependence, ruling out spin freezing. Inelastic neutron scattering data on γ-BCPO is compared with linear spin wave theory, and two separate parameter regions of the XXZ J 1 -J 2 -J 3 model with ferromagnetic nearest-neighbor exchange J 1 are favored, both near regions of high classical degeneracy. High energy coherent excitations (~10 meV) persist up to at least 40 K, suggesting strong in-plane correlations persist above TN. Finally, these data show that γ-BCPO is a rare highly frustrated, quasi-2D S eff =1/2 honeycomb lattice material which resists long range magnetic order and spin freezing.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Polarized neutron scattering study of the multiple order parameter system NdB 4 [Polarized neutron scattering study on multiple order parameter system NdB 4 ]

Neutron polarization analysis has been carried out in order to clarify the magnetic structures of multiple order parameter f-electron system NdB 4 . We confirmed the noncollinear “all-in all-out” structure (Γ 4 ) of the in-plane moment, which is in good agreement with our previous neutron powder diffraction study. We found that the magnetic moment along the c-axis m c showed diagonally antiferromagnetic structure (Γ 10 ), inconsistent with previously reported “vortex” structure (Γ 2 ). The microscopic mixture of these two structures with → q 0 =(0,0,0) appears in phase II and remains stable in phases III and IV, where an incommensurate modulation coexists. The unusual magnetic ordering is phenomenologically understood via Landau theory with the primary order parameter Γ 4 coupled with higher-order secondary order parameter Γ 10 . The magnetic moments were estimated to be 1.8 ± 0.2 and 0.2 ± 0.05μ B at T = 7.5K for Γ 4 and Γ 10 , respectively. We also found a long-period incommensurate modulation of the → q 1 =(0,0,1/2) antiferromagnetic structure of mc with the propagation → q s1 =(0.14,0.14,0.1) and → q s2 =(0.2,0,0.1) in phase III and IV, respectively. The amplitude of sinusoidal modulation was about m c =1.0 ± 0.2μ B at T=1.5 K. The local (0,0,1/2) structure consists of in-plane ferromagnetic and out-of-plane antiferromagnetic coupling of m c , opposite to the coexisting Γ 10 . The mc of Γ 10 is significantly enhanced up to 0.6μ B at T=1.5 K, which is accompanied by the incommensurate modulations. As a result, the Landau phenomenological approach indicates that the higher-order magnetic and/or multipole interactions based on the pseudoquartet f-electron state play important roles.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Tuning magnetic coercivity with external pressure in iron-rhenium based ferrimagnetic double perovskites

We studied the effect of physical pressure on the electronic and magnetic properties of ferrimagnetic double perovskites A 2 FeReO 6 (A = Ca, Ba) using Re L 2,3 edge x-ray absorption spectroscopy and powder diffraction measurements. Volume compression is shown to dramatically increase the magnetic coercivity (H c ) in polycrystalline samples of both compounds with ΔH c /ΔV similar to 150-200 Oe/Å 3 . A nearly eight-fold increase in H c , from 0.2 to 1.55 T, is obtained in Ba 2 FeReO 6 at P = 29 GPa. While no signs of structural phase transitions are seen in either sample to similar to 30 GPa, the structural data points to a pressure-driven increase in tetragonal distortion of ReO 6 octahedra. A sizable but pressure-independent Re orbital-to-spin magnetic moment ratio is observed, pointing to the critical role of spin-orbit interactions at Re sites. We present a J(eff) description of the electronic structure that combines effects of crystal field and spin-orbit coupling on the Re 5d 2 orbitals and use this description to provide insight into the pressure-induced enhancement of magnetic anisotropy.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Spin freezing into a disordered state in CaFeT i 2 O 6 synthesized under high pressure

Double perovskites exhibit a variety of interesting phenomena due to numerous combinations of cation orderings and distortions. CaMnTi 2 O 6 and CaFeTi 2 O 6 are the only two discovered double perovskites that have the columnar type A-site ordering associated with the a + a + c – titling system. The former perovskite, synthesized recently, has a polar structure below T c and shows an unusual ferroelectricity. The latter, while synthesized decades ago, received less investigation. Here, we have synthesized CaFeTi 2 O 6 under high pressure and carried out thorough characterizations through measurements of x-ray powder diffraction (XRD), second harmonic generation (SHG), dc and ac magnetization, Mössbauer spectra, resistivity, thermoelectric power, and specific heat. Although the structural refinement of the XRD pattern cannot distinguish two possible tetragonal phases, SHG measurements help to rule out the possibility of a polar structure observed in CaMnTi 2 O 6 . Fitting the paramagnetic susceptibility to a Curie-Weiss law gives a negligible Weiss constant. The weak exchange interaction gives way to a dipole-dipole interaction and single-ion anisotropy. An anomaly at 1.2 K in the specific heat is too broad for a magnetic transition, but suggestive of a spin-ice-like state as in the pyrochlores. Mössbauer spectroscopy shows two distinct iron sites, as expected for the crystal structure. Both sites are occupied by high-spin Fe 2+ as indicated by the isomer shift. The sharply different temperature dependence of the quadrupole splitting at the two iron sites can be well explained based on the local structural distortions from the refinement of XRD patterns. In conclusion, the line broadening associated with long spin-relaxation times is observed at 6 K as the spin freezing transition is approached from high temperatures.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Pressure-induced modifications of the magnetic order in the spin-chain compound C a 3 C o 2 O 6

The structural and magnetic properties of the Ca 3 Co 2 O 6 spin-chain compound have been studied by means of neutron and x-ray powder diffraction at pressures up to 6.8 and 32 GPa, respectively. A suppression of the initial spin-density wave state (T N = 25 K) and stabilization of the collinear commensurate antiferromagnetic (AFM) state at high pressures (T NC = 26 K at P = 2.1 GPa) were observed. The pressure behavior of the competing intra- and interchain magnetic interactions was analyzed on the basis of obtained structural data and their role in the formation of the magnetic phase diagram is discussed. Here, the pressure behavior of the Néel temperature of the commensurate AFM phase was evaluated within the mean field theory approach and a good agreement with the experimental value dT NC /dP = 0.65 K/GPa was obtained.

1-dimensional spin chains↗
DOE OSTI2018

Emphanitic anharmonicity in PbSe at high temperature and anomalous electronic properties in the Pb Q ( Q = S , Se , Te ) system

Here, the temperature dependence of the local structure of PbSe has been investigated using pair distribution function (PDF) analysis of x-ray and neutron powder diffraction data and density functional theory (DFT) calculations. Observation of non-Gaussian PDF peaks at high temperature indicates the presence of significant anharmonicity, which can be modeled as Pb off-centering along [100] directions that grows on warming similar to the behavior seen in PbTe and PbS and sometimes called emphanisis. Interestingly, the emphanitic response is smaller in PbSe than in both PbS and PbTe indicating a nonmonotonic response with chalcogen atomic number in the PbQ (Q = S, Se, Te) series. The DFT calculations indicate a correlation between band gap and the amplitude of [100] dipolar distortion, suggesting that emphanisis may be behind the anomalous composition and temperature dependencies of the band gaps in this series.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Revisiting the Kitaev material candidacy of Ir 4 + double perovskite iridates

Quantum magnets with significant bond-directional Ising interactions, so-called Kitaev materials, have attracted tremendous attention recently in the search for exotic spin liquid states. Here we present a comprehensive set of measurements that enables us to investigate the crystal structures, Ir 4+ single-ion properties, and magnetic ground states of the double perovskite iridates La 2 BIrO 6 (B = Mg, Zn) and A 2 CeIrO 6 (A = Ba, Sr) with a large nearest-neighbor distance >5 angstrom between Ir 4+ ions. Our neutron powder diffraction data on Ba 2 CeIrO 6 can be refined in the cubic space group Fm$\overline{3}$m, while the other three systems are characterized by weak monoclinic structural distortions. Despite the variance in the noncubic crystal field experienced by the Ir 4+ ions in these materials, x-ray absorption spectroscopy and resonant inelastic x-ray scattering are consistent with J eff = 1/2 moments in all cases. Furthermore, neutron scattering and resonant magnetic x-ray scattering show that these systems host A-type antiferromagnetic order. These electronic and magnetic ground states are consistent with expectations for face-centered-cubic magnets with significant antiferromagnetic Kitaev exchange, which indicates that spacing magnetic ions far apart may be a promising design principle for uncovering additional Kitaev materials

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

High Pressure Synthesis of Rubidium Superhydrides

Through laser-heated diamond anvil cell experiments, we synthesize a series of rubidium superhydrides and explore their properties with synchrotron x-ray powder diffraction and Raman spectroscopy measurements, combined with density functional theory calculations. Upon heating rubidium monohydride embedded in H 2 at a pressure of 18 GPa, we form RbH 9 − I , which is stable upon decompression down to 8.7 GPa, the lowest stability pressure of any known superhydride. At 22 GPa, another polymorph, RbH 9 − II is synthesised at high temperature. Unique to the Rb-H system among binary metal hydrides is that further compression does not promote the formation of polyhydrides with higher hydrogen content. Instead, heating above 87 GPa yields RbH 5 , which exhibits two polymorphs ( RbH 5 − I and RbH 5 − II ). All of the crystal structures comprise a complex network of quasimolecular H 2 units and H − anions, with RbH 5 providing the first experimental evidence of linear H 3 − anions. Published by the American Physical Society 2025

Kuzovnikov, Mikhail A.↗
DOE OSTI2019

Steplike metamagnetic transitions in a honeycomb lattice antiferromagnet Tb 2 Ir 3 Ga 9

Single crystals of a honeycomb lattice antiferromagnet, Tb 2 Ir 3 Ga 9 , were synthesized, and the physical properties have been studied. From magnetometry, a long-range antiferromagnetic ordering at ≈12.5 K with highly anisotropic magnetic behavior was found. Neutron powder diffraction confirms that the Tb spins lie along the a-axis, parallel to the shortest Tb-Tb contact. Two field-induced spin-flip transitions are observed when the field is applied parallel to this axis, separated by a plateau corresponding roughly to M ≈ M s /2. Transport measurements show the resistivity to be metallic with a discontinuity at the onset of Néel order. Heat capacity shows a λ-like transition confirming the bulk nature of the magnetism.We propose a phenomenological spin Hamiltonian that describes the magnetization plateau as a result of strong Ising character arising from a quasidoublet ground state of the Tb 3+ ion in a site of C s symmetry and expressing a significant bond-dependent anisotropy.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Tunable magnetic order in low-symmetry SeO 3 ligand linked TM 3 (SeO 3 ) 3 H 2 O ( TM =Mn , Co, and Ni) compounds

The ability to design crystal lattices with specific sublattice geometries has long been sought after especially in the context of harnessing magnetic frustration to elicit emergent physics. One approach which has seen some success recently is to design magnetic sublattices chemically through the use of nonmagnetic linker ligands as scaffolding for the magnetic ions. In this work we report the magnetic properties of one such family of materials, the transition metal (TM) selenite hydrates with chemical formula TM 3 (SeO 3 ) 3 H 2 O. These materials link highly distorted TMO 6 octahedra via nonmagnetic [SeO 3 ] 2+ linkers. Studying members with TM = Mn, Co, and Ni we use magnetic susceptibility and neutron powder diffraction to identify antiferromagnetic order in all three compounds with moderate frustration indexes. A comparison of the magnetic structures suggests that while the overall structure of the SeO 3 scaffolding remains unchanged the TM effects changes in the magnetic properties through tuning the internal bonding parameters and the single-ion physics. Changing from Mn to Co is found to be particularly consequential manifesting changes in both the ordered-moment direction and in the direction of the ordering vector. Field-dependent measurements of the susceptibility and heat capacity reveal metamagnetic transitions in both Mn 3 (SeO 3 ) 3 H 2 O and Co 3 (SeO 3 ) 3 H 2 O indicating nearby magnetic ground states accessible under relatively small applied fields. Density functional theory calculations broadly confirm these results, showing both a sensitivity of the magnetic structure to the TM and its local environment. Although no spin liquid behavior is achieved, these results suggest the fruitfulness of such synthesis philosophies and encourage future work to engender higher frustration in these materials via doping, field, pressure, or larger linker ligands.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Evolution of noncollinear magnetism in magnetocaloric MnPtGa

MnPtGa crystallizes in the hexagonal Ni 2 In structure type in space group P6 3 /mmc and has been reported to display a ferromagnetic Curie temperature near 220K. Here we find a transition near T c = 236 K to a ferromagnetic state, albeit with a reduced moment from what is expected for collinear ordering. The peak magnetocaloric entropy change was determined to be ΔS M = –1.9 J kg –1 K –1 for an applied magnetic field of H = 5 T at the ferromagnetic ordering temperature. Magnetostructural coupling manifests as a change in the slope of the thermal expansion coefficients of the c lattice parameter near T c , with a negative spontaneous volume magnetostriction; ω = –300 ppm at 190K. In this work, neutron powder diffraction studies of the magnetic ground state reveal an evolution in complexity as temperature decreases: from a ferromagnet, to a canted antiferromagnet, to the eventual formation of a spin-density-wave state at low temperatures.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Complex magnetic properties in the mixed 4 f - 5 d double perovskite iridates X 2 ZnIrO 6 ( X = Nd , Sm , Eu , Gd )

Here in this paper, we report on the synthesis and magnetic properties of a series of double perovskites Ln 2 ZnIrO 6 with Ln = Nd, Sm, Eu, Gd. These compounds present examples of the rare case of double perovskites (general formula A 2 BB'O6) with a magnetic 4ƒ-ion on the A site in combination with the strongly spin-orbit coupled 5d transition-metal ion Ir 4+ on the B sublattice. We discuss the impact of different rare earths on the macroscopic magnetic properties. Gd 2 ZnIrO 6 and Eu 2 ZnIrO 6 show ferrimagnetic or canted antiferromagnetic order below T N = 23 and 12 K, respectively. Sm 2 ZnIrO 6 orders antiferromagnetically at T N = 13 K. Nd 2 ZnIrO 6 exhibits more complex magnetic properties with a strong field dependence ranging from a two-step spin reorientation at μ 0 H = 0.01 T to an antiferromagnetic ground state at intermediate external fields to a spin-flop phase for 0H ≥ 4 T. This unique behavior suggests an interesting interplay between Nd 3+ and Ir 4+ . To further shed light on the relevant magnetic interaction, the zero-field magnetic ground state of Nd 2 ZnIrO 6 is examined via neutron powder diffraction. In general, the magnetic properties of Ln 2 ZnIrO 6 hint towards a substantial contribution of the rare-earth ions and a significant correlation between 5d and 4ƒ magnetism.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Canted antiferromagnetic order in the monoaxial chiral magnets V 1/3 TaS 2 and V 1/3 NbS 2

The Dzyaloshinskii-Moriya (DM) interaction is present in the transition metal dichalcogenides (TMDC) magnets of form M 1 / 3 T S 2 ( M = 3 d transition metal, T ϵ { Nb , Ta } ), given that the intercalants M form 3 × 3 superlattices within the structure of the parent materials T S 2 and break the centrosymmetry. Competition between DM and ferromagnetic exchange interactions has been shown to stabilize a topological defect known as a chiral soliton in select intercalated TMDCs, initiating interest both in terms of fundamental physics and the potential for technological applications. In the current article we report on our study of the materials V 1 / 3 TaS 2 and V 1 / 3 NbS 2 , using a combination of x-ray powder diffraction, magnetization, and single crystal neutron diffraction. Historically identified as ferromagnets, our diffraction results instead reveal that vanadium spins in these compounds are arranged into an A-type antiferromagnetic configuration at low temperatures. Refined moments are 1.37(6) and 1.50(9) μ B for V 1 / 3 TaS 2 and V 1 / 3 NbS 2 , respectively. Transition temperatures T c = 32 K for V 1 / 3 TaS 2 and 50 K for V 1 / 3 NbS 2 are obtained from the magnetization and neutron diffraction results. We attribute the small net magnetization observed in the low-temperature phases to a subtle ( ~ 2 ° ) canting of XY spins in the out-of-plane direction. These new results are indicative of dominant antiferromagnetic exchange interactions between the vanadium moments in adjacent a b planes, likely eliminating the possibility of identifying stable chiral solitons in the current materials.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Magnetoelectric effect arising from a field-induced pseudo Jahn-Teller distortion in a rare-earth magnet

Magnetoelectric materials are attractive for several applications, including actuators, switches, and magnetic field sensors. Typical mechanisms for achieving a strong magnetoelectric coupling are rooted in transition metal magnetism. In sharp contrast, here we identify CsEr(MoO 4 ) 2 as a magnetoelectric material without magnetic transition metal ions, thus ensuring that the Er ions play a key role in achieving this interesting property. Our detailed study includes measurements of the structural, magnetic, and magnetoelectric properties of this material. Bulk characterization and neutron powder diffraction show no evidence for structural phase transitions down to 0.3 K and therefore CsEr(MoO 4 ) 2 maintains the room temperature P2/c space group over a wide temperature range without external magnetic field. These same measurements also identify collinear antiferromagnetic ordering of the Er 3+ moments below T N =0.87K. Complementary dielectric constant and pyroelectric current measurements reveal that a ferroelectric phase with a maximum polarization P~0.6 nC/cm 2 emerges when applying a modest external magnetic field, which indicates that this material has a strong magnetoelectric coupling. Finally, we argue that the magnetoelectric coupling in this system arises from a pseudo Jahn-Teller distortion induced by the magnetic field.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Competing magnetic states in multiferroic BaYFeO 4 : A high magnetic field study

Spin-driven ferroelectricity phenomena have drawn great interest in the scientific community due to potential application in spintronics and their complex physical mechanisms. A noticeable example of this is multiferroic BaYFeO 4 that exhibits an unconventional magnetoelectric (ME) coupling due to the uncorrelated behavior of the ferroelectric and cycloidal states under an applied magnetic field. To shed more light on this spin-driven ME effect, a high-quality sample of BaYFeO 4 was synthesized by a standard solid-state reaction method, and its high-field (up to 9 T) magnetic properties have been systematically investigated by means of magnetometry, magnetocaloric effect, and Mössbauer measurements over a wide temperature range (5–400 K). In addition, its crystal and magnetic structures have been studied using x-ray and neutron powder diffraction. Results obtained in this work indicate that Fe spins form a long-range spin density wave (SDW) antiferromagnetic (AFM) order at $T_{\text{N1}}$ ~ 50K, which transforms into the cycloidal AFM order at $T_{\text{N2}}$ ~ 35K. A spin-glass-like state emerges below $T^\ast$ ~ 17K, and coexists with the long-range cycloidal AFM one in this temperature range. Magnetocaloric and Mössbauer measurements consistently confirm the robustness of both the long-range SDWand cycloidal AFM orders under applied magnetic fields up to 6 T, whereas the spin-glass state is converted into the ferromagnetic (FM) state when the applied magnetic field exceeds 1 T. These findings pinpoint the fact that the magnetic field evolution of spin correlations from the AFM to FM character in the spin-glass state is responsible for the magnetic field dependence of ferroelectricity in BaYFeO 4 .

36 MATERIALS SCIENCE↗
DOE OSTI2021

Relationship between A-site cation and magnetic structure in 3d–5d–4f double perovskite iridates Ln 2 NiIrO 6 ( Ln = La, Pr, Nd)

We report a comprehensive investigation of Ln 2 NiIrO 6 (Ln=La, Pr, Nd) using thermodynamic and transport properties, neutron powder diffraction, resonant inelastic x-ray scattering, and density-functional theory (DFT) calculations to investigate the role of A-site cations on the magnetic interactions in this family of hybrid 3d–5d–4f compositions. Magnetic structure determination using neutron diffraction reveals antiferromagnetism for La 2 NiIrO 6 , a collinear ferrimagnetic Ni and Ir state that is driven to long-range antiferromagnetism upon the onset of Nd ordering in Nd 2 NiIrO 6 , and a noncollinear ferrimagnetic Ni and Ir sublattice interpenetrated by a ferromagnetic Pr lattice for Pr 2 NiIrO 6 . For Pr 2 NiIrO 6 , heat-capacity results reveal the presence of two independent magnetic sublattices, and transport resistivity indicates insulating behavior and a conduction pathway that is thermally mediated. Here, a first principles DFT calculation elucidates the existence of the two independent magnetic sublattices within Pr 2 NiIrO 6 and offers insight into the behavior in La 2 NiIrO 6 and Nd 2 NiIrO 6 . Resonant inelastic x-ray scattering is consistent with spin-orbit coupling splitting the t 2 g manifold of octahedral Ir 4+ into a J eff = 1/2 and J eff = 3/2 state for all members of the series considered.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Helical versus collinear antiferromagnetic order tuned by magnetic anisotropy in polar and chiral (Ni,Mn) 3 TeO 6

In this work, polar and chiral Ni 3 TeO 6 was found to exhibit a colossal magnetoelectric (ME) effect associated with collinear antiferromagnetic order. We have investigated the evolution of its magnetic state with the substitution of the Ni 2+ spins by isotropic Mn 2+ spins, namely (Ni, Mn) 3 TeO 6 (NMTO). The ground state of NMTO maintains an Ising nature, but a new phase with XY-type magnetic anisotropy is discovered at an intermediate temperature range. Neutron powder diffraction experiments reveal that (1) Mn ions tend to occupy a specific transition-metal site, consistent with the first-principle calculation, and (2) the intermediate phase is an incommensurate (IC) helical magnetic state propagating along the $\textit{c}$ axis with $\vec q_{\text{IC}}$ = (0, 0, 1.5 ± δ). We also found that the balance between these two magnetic states can be readily manipulated with magnetic fields, which results in significant ME effects. This selective site occupancy of NMTO allows for a unique competition between collinear and helical magnetic structures with minimal chemical disorder. Thus, NMTO serves as a model system to study site-specific chemical control of noncollinear magnetism and ME coupling.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Temperature-induced valence-state transition in double perovskite Ba 2 - x Sr x TbIrO 6

In this paper, a temperature-induced valence-state transition is studied in a narrow composition range 0.2 ≤ x ≤ 0.375 of Ba 2 - x Sr x TbIrO 6 by means of x-ray and neutron powder diffraction, resonant inelastic x-ray scattering, magnetic susceptibility, electrical resistivity, and specific heat measurements. The valence-state transition involves an electron transfer between Tb and Ir leading to the valence-state change between Tb 3 + / Ir 5 + and Tb 4 + / Ir 4 + phases. This first-order transition has a dramatic effect on the lattice, transport properties, and the long-range magnetic order at low temperatures for both Tb and Ir ions. Ir 5 + ion has an electronic configuration of 5 d 4 ( J eff = 0 ), which is expected to be nonmagnetic. In contrast, Ir 4 + ion with a configuration of 5 d 5 ( J eff = 1/2) favors a long-range magnetic order. For x = 0.1 with Tb 3 + / Ir 5 + configuration to the lowest temperature (2 K) investigated in this paper, a spin-glass behavior is observed around 5 K indicating Ir 5 + ( J eff = 0 ) ions act as a spacer reducing the magnetic interactions between Tb 3 + ions. For x = 0.5 with Tb 4 + / Ir 4 + configuration below the highest temperature 400 K of this paper, a long-range antiferromagnetic order at T N = 40 K is observed highlighting the importance of Ir 4 + ( J eff = 1/2) ions in promoting the long-range magnetic order of both Tb and Ir ions. For 0.2 ≤ x ≤ 0.375, a temperature-induced valence-state transition from high-temperature Tb 3 + / Ir 5 + phase to low-temperature Tb 4 + / Ir 4 + phase occurs in the temperature range 180 K ≤ T ≤ 325 K and the transition temperature increases with x . The compositional dependence demonstrates the ability to tune the the valence state for a critical region of x that leads to a concurrent change in magnetism and structure. Furthermore, this tuning ability could be employed with suitable strain in thin films to act as a switch as the magnetism is manipulated.

36 MATERIALS SCIENCE↗