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At least 955 records · Page 53

Spin-selective evolution of the Zhang-Rice state in binary transition metal oxide MnO(001) film

Here, the Zhang-Rice (ZR) state is a strongly hybridized bound state formed by transition-metal and oxygen atoms. The spin fluctuations within the ZR state are known to play an important role in high-T c superconductivity in cuprates. Here, we employ a combination of angle-resolved photoemission spectroscopy (ARPES), x-ray photoemission spectroscopy (XPS), and ab initio embedded dynamical mean-field theory (eDMFT) to investigate the influence of magnetic ordering on the spectral characteristics of the valence band and Mn 2⁢p core-level in MnO (001) ultrathin films. Our results demonstrate that a complex spin-selective evolution of Mn 3⁢d-O2⁢p hybridization develops due to the long-range antiferromagnetic (AFM) ordering. This hybridization significantly alters the spectral shape and weight of the ZR state. Specifically, in the AFM phase, we observed the sharpening of the ZR state and band folding with the periodicity of the AFM unit cell of MnO(001). We also demonstrated a strong connection between the spectral evolution of the ZR state and the non-local screening channels of the photoexcited core holes. Further, our detailed temperature-dependent study reveals the presence of short-range antiferromagnetic correlations that exist at much higher temperatures than Neel temperature (T N ) and shows the evolution of the ZR state across the magnetic transitions and its implication to the core-hole screening in 3⁢d binary transition metal oxides.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Frustration-mediated crossover from long-range to short-range magnetic ordering in Y 1 – x L u x BaC o 4 O 7

The R⁢BaC⁢o 4⁢ O 7 system is a prototype geometrically frustrated magnet in which kagome planes and triangular layers of Co-O tetrahedra interleave. For R=Y, an antiferromagnetic ground state is realized due to a frustration-breaking trigonal-orthorhombic phase transition. For R = Lu, however, a long-range ordered state has rarely, if ever, been reported despite a similar symmetry-breaking transition, albeit at a significantly lower temperature. To explore this dichotomy, we present a comprehensive magnetic and structural phase diagram for Y 1-x L⁢u x BaC⁢o 4 ⁢O 7 , established through complementary neutron diffraction and magnetization measurements. Our results outline the phase evolution of the nuclear structures in response to changes in composition and temperature. Further, the temperature of the trigonal (P⁢31⁢c) to orthorhombic (Pbn⁢2 1 ) transition, T s⁢1 , decreases monotonically with increasing Lu content from 310 K for x = 0.0 to 110 K for x = 1.0. In Lu-rich compositions (0.7 ≤ x ≤ 1.0), first-order structural transitions are observed with coexisting and competing orthorhombic Pbn⁢2 1 and metastable monoclinic Cc phases. For the magnetically ordered Y-rich compositions, T- and x-dependent refinements of the magnetic structure reveal an antiferromagnetic “ribbonlike” arrangement of Co spin pairs in both the triangular and the kagome layers. A gradual suppression of long-range magnetic order is observed with increasing the Lu content, accompanied by the development of short-range magnetic correlations present in all the samples.

36 MATERIALS SCIENCE↗

Electronic and magnetic structures of a mixed triple perovskite: Ba 3 NiRuIrO 9

In search of spin-orbit coupling driven nonmagnetic J = 0 ground state and excitonic magnetism, various pentavalent iridates have been studied in recent years. However, a finite moment was observed in most of the cases due to solid state effects. Here, in this work, we investigate the electronic and magnetic structure of 6H hexagonal compound Ba 3 NiRuIrO 9 , where Ir 5+ is present along with magnetic Ni 2+ and Ru 5+ ions. Magnetic susceptibility measurements and neutron powder diffraction (NPD) experiments demonstrate the appearance of short-range magnetic ordering below 170 K and a long-range antiferromagnetic ordering below 80 K. The refinement of the NPD pattern further shows that the Ru and Ir moments interact antiferromagnetically within the dimer and interact ferromagnetically with the Ni sublattice. These experimental findings have been complemented by first-principles density functional theory calculations incorporating spin-orbit coupling effects and electronic correlations for the transitional metal d states. The computed magnetocrystalline anisotropy is also found to be significant and the crystallographic c axis comes out to be the easy axis of magnetization, consistent with the spin alignment direction found from NPD. This study shows that the mixed ruthenate iridate triple perovskite series is a promising family to study the interplay among spin-orbit coupling, electron correlation, and electron filling as a variety of Ba 3 M RuIrO 9 with M as a transition metal ion, rare-earth ion, and alkali metal ions can be synthesized.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Linking NH$^+_4$ motion to magnetism in molecular multiferroic (NH 4 ) 2 ⁢[FeCl 5 ⁢(H 2 ⁢O)]: A neutron vibrational spectroscopy study

Here, we present a neutron vibrational spectroscopy study to investigate the influence of NH$^+_4$ motion on the magnetism in [(NH 4 ) 1–x K x ] 2 ⁢[FeCl 5 ⁢(H 2 ⁢O)]. The parent compounds, (NH 4 ) 2 ⁢[FeCl 5 ⁢(H 2 ⁢O)] (x = 0) and K 2 ⁡[FeCl 5 ⁢(H 2 ⁢O)]⁢(x = 1) are isostructural at room temperature, yet displaying drastically different magnetic and multiferroic behavior. K 2 ⁡[FeCl 5 ⁢(H 2 ⁢O)] is nonmultiferroic with type-A collinear antiferromagnetic structure below T N ≈ 14.06 K, whereas (NH 4 ) 2 ⁢[FeCl 5 ⁢(H 2 ⁢O)] is a type-II multiferroic with incommensurate cycloidal spin structure below T FE ≈ 6.8 K. A recent study of the dielectric, structure, and magnetic properties in the mixed [(NH 4 ) 1–x ⁢K x ] 2 ⁢[FeCl 5 ⁢(H 2 ⁢O)] shows that a small amount of potassium substitution to replace NH$^+_4$ transforms the spin structure from incommensurate cycloidal (x ≤ 0.06) into commensurate collinear antiferromagnetic (x ≥ 0.15), indicating NH$^+_4$ is essential to the emergent phenomena observed in this molecular multiferroic compound. Our vibrational spectroscopy study reveals that NH$^+_4$ libration and torsion motion exhibit substantial temperature dependence at low temperatures. The intensity of NH$^+_4$ libration and torsion modes increases slightly at 5 K in comparison with data at 25 K behaving like a magnon, indicating that they are coupled to the magnetism in (NH 4 ) 2 ⁢[FeCl 5 ⁢(H 2 ⁢O)]. Comparing data of x=0, 0.06, 0.09, and 0.15 samples further illustrates that the strength of the increased signal in NH$^+_4$ libration mode is very sensitive to potassium concentration. The signal diminishes quickly with increasing potassium concentration and vanishes in the x = 0.15 sample corresponding to the magnetic structure change for x ≥ 0.15. The results directly link the anomalous behavior in NH$^+_4$ libration motion to the magnetism in [(NH 4 ) 1–x ⁢K x ] 2 ⁢[FeCl 5 ⁢(H 2 ⁢O)], providing new insights into the crucial role NH$^+_4$ plays in the coupled phenomena in (NH 4 ) 2 ⁢[FeCl 5 ⁢(H 2 ⁢O)]. The unique information opens a new door to go through in searching for new multifunctional materials by incorporation of NH 4 via a material-by-design approach.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Anisotropic excitonic magnetism from discrete C 4 symmetry in CeRhIn 5

Anisotropy in strongly correlated materials is a central parameter in determining the electronic ground state and is tuned through the local crystalline electric field. This is notably the case in the CeCo x Rh 1 − x In 5 system where the ground-state wave function can provide the basis for antiferromagnetism and/or unconventional superconductivity. We develop a methodology to understand the local magnetic anisotropy and experimentally investigate with neutron spectroscopy applied to antiferromagnetic ( T N = 3.8 K ) CeRhIn 5 , which is isostructural to d -wave superconducting ( T c = 2.3 K ) CeCoIn 5 . Through diagonalizing the local crystal field Hamiltonian with discrete tetragonal C 4 point group symmetry and coupling these states with the random phase approximation, we find two distinct modes polarized along the crystallographic c and a − b planes, agreeing with experiment. The anisotropy and bandwidth, underlying the energy scale of these modes, are tuneable with a magnetic field which we use experimentally to separate in energy single and multiparticle excitations thereby demonstrating the instability of excitations polarized within the crystallographic a − b plane in CeRhIn 5 . We compare this approach to a S eff = 1 2 parametrizations and argue for the need to extend conventional SU(2) theories of magnetic excitations to utilize the multilevel nature of the underlying crystal-field basis states constrained by the local point-group C 4 symmetry. Published by the American Physical Society 2024

Brener, D. J. (ORCID:0000000333400177)↗

Effect of Ni substitution on the fragile magnetic system La 5 Co 2 Ge 3

La 5⁢ Co 2 ⁢Ge 3 is an itinerant ferromagnet with a Curie temperature T C of ~3.8K and a remarkably small saturated moment of 0.1µ B /Co. Here we present the growth and characterization of single crystals of the La 5 ⁢(Co 1–x⁢ Ni x ) 2 Ge 3 series for 0.00 ≤ x ≤ 0.186. Here we measured powder x-ray diffraction, composition as well as anisotropic temperature-dependent resistivity, temperature and field-dependent magnetization along with heat capacity on these single crystals. We also measured muon-spin rotation/relaxation (μ⁢SR) for some Ni substitutions (x = 0.027,0.036,0.074) to study the evolution of internal field with Ni substitution. Using the measured data we infer a low temperature, transition temperature-composition phase diagram for La 5 ⁢(Co 1–x ⁢Ni x ) 2 Ge 3 . We find that T C is suppressed for low dopings, x ≤ 0.014; whereas for 0.036 ≤ x ≤ 0.186, the samples are antiferromagnetic with a Néel temperature T N that goes through a weak and shallow maximum (T N ~ 3.4K for x~0.07) and then gradually decreases to 2.4 K by x = 0.186. For intermediate Ni substitutions, 0.016 ≤ x ≤ 0.027, two transition temperatures are inferred with T N >T C . Whereas the T–x phase diagram for La 5 ⁢(Co 1–x ⁢Ni x ) 2 Ge 3 and the T–p phase diagram determined for the parent La 5 ⁢Co 2 ⁢Ge 3 under hydrostatic pressure are grossly similar, changing from a low-doping or low-pressure ferromagnetic (FM) ground state to a high-doped or high-pressure antiferromagnetic (AFM) state, perturbation by Ni substitution enabled us to identify an intermediate doping regime where both FM and AFM transitions occur.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Long-range magnetic order induced surface state in GdBi and DyBi

The recent discovery of unconventional surface-state pairs, which give rise to Fermi arcs and spin textures, in antiferromagnetically ordered rare-earth monopnictides attracted the interest in these materials. Here, we use angle-resolved photoemission spectroscopy measurements in conjunction with density functional theory calculations to investigate the evolution of the electronic structure of GdBi and DyBi. We find that new surface states, including a Dirac cone, emerge in the antiferromagnetic (AFM) state. However, they are located along a direction in momentum space that is different than what was found in NdSb, NdBi, and CeBi. The observed changes in the electronic structure are consistent with the presence of AFM-II-A type order.

36 MATERIALS SCIENCE↗

Long-lived oscillations of metastable states in neutral atom systems

Metastable states arise in a range of quantum systems and can be observed in various dynamical scenarios, including decay, bubble nucleation, and long-lived oscillations. The phenomenology of metastable states has been examined in quantum many-body systems, notably in one-dimensional (1D) ferromagnetic Ising spin systems and superfluids. Here, in this paper, we study long-lived oscillations of metastable and ground states in 1D antiferromagnetic neutral atom chains with long-range Rydberg interactions. We use a staggered local detuning field to achieve confinement. Using theoretical and numerical models, we identify novel spectral signatures of quasiparticle oscillations distinct to antiferromagnetic neutral atom systems and interpret them using a classical energy model of short-range meson repulsion. Finally, we evaluate the experimental accessibility of our proposed setup on current neutral-Atom platforms and discuss experimental feasibility and constraints.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Structural and magnetic characterization of CeTa 7 ⁢O 19 and YbTa 7 ⁢ O 19 with a two-dimensional pseudospin-$\frac{1}{2}$ triangular lattice

Triangular lattice antiferromagnets are prototypes for frustrated magnetism and may potentially realize novel quantum magnetic states such as a quantum spin-liquid ground state. A recent work suggests NdTa 7 ⁢O 19 with rare-earth triangular lattice is a quantum spin-liquid candidate and highlights the large family of rare-earth heptatantalates as a framework for quantum magnetism investigation. Here, in this paper, we report the structural and magnetic characterization of CeTa 7 ⁢ O 19 and YbTa 7 ⁢ O 19 . Both compounds are isostructural to NdTa 7 ⁢O 19 with no detectable structural disorder. For CeTa 7 ⁢O 19 , the crystal field energy levels and parameters are determined by inelastic neutron scattering measurements. Based on the crystal field result, the magnetic susceptibility data could be well fitted and explained, which reveals that CeTa 7 ⁢O 19 is a highly anisotropic Ising triangular-lattice antiferromagnet (𝑔 𝑧 ⁡/𝑔 𝑥⁢𝑦 ∼ 3) with very weak exchange interaction (J ∼ 0.22 K). For YbTa 7⁢ O 19 , millimeter-sized single crystals could be grown. The anisotropic magnetization and electron spin resonance data show that YbTa 7⁢ O 19 has a contrasting in-plane magnetic anisotropy with 𝑔 𝑧 ⁡/𝑔 𝑥⁢𝑦 ∼ 0.67 similar as that of YbMgGaO 4 . The above results indicate that CeTa7⁢ O 19 and YbTa 7 ⁢O 19 with pseudospin-1/2 ground states might either be quantum spin-liquid candidate materials or find applications in adiabatic demagnetization refrigeration due to the weak exchange interaction.

Pan, Feihao↗

Magnetic properties of a staggered S = 1 chain with an alternating single-ion anisotropy direction

Materials composed of spin-1 antiferromagnetic (AFM) chains are known to adopt complex ground states that are sensitive to the single-ion-anisotropy (SIA) energy ( D ), and intrachain ( J 0 ) and interchain ( J 1 , 2 ′ ) exchange energy scales. While theoretical and experimental studies have extended this model to include various other energy scales, the effect of the lack of a common SIA axis is not well explored. Here we investigate the magnetic properties of Ni ( pyrimidine ) ( H 2 O ) 2 ( NO 3 ) 2 , a chain compound where the tilting of Ni octahedra leads to a twofold alternation of the easy-axis directions along the chain. Muon-spin relaxation measurements indicate a transition to long-range order at T N = 2.3 K and the magnetic structure is initially determined to be antiferromagnetic and collinear using elastic neutron diffraction experiments. Inelastic neutron scattering measurements were used to find J 0 = 5.107 ( 7 ) K , D = 2.79 ( 1 ) K , J 1 ′ = 0.00 ( 5 ) K , J 2 ′ = 0.18 ( 3 ) K , and a rhombic anisotropy energy E = 0.19 ( 9 ) K . Mean-field modeling reveals that the ground state structure hosts spin canting of ϕ ≈ 6 . 5 ∘ , which is not detectable above the noise floor of the elastic neutron diffraction data. Monte Carlo simulation of the powder-averaged magnetization, M ( H ) , is then used to confirm these Hamiltonian parameters, while single-crystal M ( H ) simulations provide insight into features observed in the data. Published by the American Physical Society 2025

Vaidya, S. (ORCID:000000033975497X)↗

Octupolar versus Néel Order in Cubic 5d 2 Double Perovskites

We report time-of-flight neutron spectroscopy and neutron and x-ray diffraction studies of the 5 d 2 double perovskite magnets, Ba 2 M OsO 6 ( M = Zn , Mg , Ca ). We find that these materials host antiferromagnetically coupled 5 d 2 Os 6 + ions decorating a face-centered cubic (fcc) lattice and are found to remain cubic down to the lowest temperatures. They all exhibit thermodynamic anomalies consistent with a single phase transition at a temperature T * , and a gapped magnetic excitation spectrum with spectral weight concentrated at wave vectors typical of type-I antiferromagnetic orders. However, while muon spin resonance experiments show clear evidence for time-reversal symmetry breaking below T * , we observe no corresponding magnetic Bragg scattering signal. These results are shown to be consistent with ferro-octupolar symmetry breaking below T * , and are discussed in the context of other 5 d double perovskite magnets and theories of exotic orders driven by multipolar interactions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Direct Evidence of the Competing Nature between Electronic and Lattice Breathing Order in Rare-Earth Nickelates

Correlated electrons give rise to both exotic electronic and magnetic properties in rare-earth nickelates. IN this research, we introduce evidence of the interfacial coupling between two nickelate systems, EuNiO 3 (ENO) and LaNiO 3 (LNO), with different electronic and magnetic properties but with compatible structural registry giving rise to an electrostructural transition, unobserved in each constituent. Nominally, LNO remains in a paramagnetic-metallic R 3 ¯ c phase while orthorhombic ENO undergoes antiferromagnetic and insulating transitions. However, the ENO/LNO heterostructure displays a uniform rotational symmetry set by an entwined interface. This leads to an anomalous reduction of bond disproportionation in the ENO layer through the metal to insulator transition and concomitantly charge disproportionation opens the gap accompanied by antiferromagnetic ordering. Our findings resolve a long-standing question in the physics of rare-earth nickelates, herein demonstrating that charge and bond disproportionation are competing mechanisms for the charge localization process in the rare-earth nickelate system.

36 MATERIALS SCIENCE↗

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↗

Modeling Unconventional Superconductivity at the Crossover between Strong and Weak Electronic Interactions

High-temperature superconductivity emerges in many different quantum materials, often in regions of the phase diagram where the electronic kinetic energy is comparable to the electron-electron repulsion. Describing such intermediate-coupling regimes has proven challenging as standard perturbative approaches are inapplicable. In this study, we employ quantum Monte Carlo methods to solve a multiband Hubbard model that does not suffer from the sign problem and in which only repulsive interband interactions are present. In contrast to previous sign-problem-free studies, we treat magnetic, superconducting, and charge degrees of freedom on an equal footing. We find an antiferromagnetic dome accompanied by a metal-to-insulator crossover line in the intermediate-coupling regime, with a smaller superconducting dome appearing in the metallic region. Across the antiferromagnetic dome, the magnetic fluctuations change from overdamped in the metallic region to propagating in the insulating region. Our findings shed new light on the intertwining between superconductivity, magnetism, and charge correlations in quantum materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Room-Temperature Ferromagnetism at an Oxide-Nitride Interface

Heterointerfaces have led to the discovery of novel electronic and magnetic states because of their strongly entangled electronic degrees of freedom. Single-phase chromium compounds always exhibit antiferromagnetism following the prediction of the Goodenough-Kanamori rules. So far, exchange coupling between chromium ions via heteroanions has not been explored and the associated quantum states are unknown. In this work, we report the successful epitaxial synthesis and characterization of chromium oxide (Cr 2 O 3 )-chromium nitride (CrN) superlattices. Room-temperature ferromagnetic spin ordering is achieved at the interfaces between these two antiferromagnets, and the magnitude of the effect decays with increasing layer thickness. First-principles calculations indicate that robust ferromagnetic spin interaction between Cr 3+ ions via anion-hybridization across the interface yields the lowest total energy. This work opens the door to fundamental understanding of the unexpected and exceptional properties of oxide-nitride interfaces and provides access to hidden phases at low-dimensional quantum heterostructures.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Discovery of Charge Order and Corresponding Edge State in Kagome Magnet FeGe

Kagome materials often host exotic quantum phases, including spin liquids, Chern gap, charge density wave, and superconductivity. Existing scanning microscopy studies of the kagome charge order have been limited to nonkagome surface layers. Here, we tunnel into the kagome lattice of FeGe to uncover features of the charge order. Our spectroscopic imaging identifies a 2×2 charge order in the magnetic kagome lattice, resembling that discovered in kagome superconductors. Spin mapping across steps of unit cell height demonstrates the existence of spin-polarized electrons with an antiferromagnetic stacking order. We further uncover the correlation between antiferromagnetism and charge order anisotropy, highlighting the unusual magnetic coupling of the charge order. Finally, we detect a pronounced edge state within the charge order energy gap, which is robust against the irregular shape fluctuations of the kagome lattice edges. Here, we discuss our results with the theoretically considered topological features of the kagome charge order including unconventional magnetism and bulk-boundary correspondence.

36 MATERIALS SCIENCE↗

Anomalous Electrical Transport in the Kagome Magnet YbFe 6 ⁢Ge 6

Two-dimensional (2D) kagome metals offer a unique platform for exploring electron correlation phenomena derived from quantum many-body effects. Here, in this study, we report a combined study of electrical magnetotransport and neutron scattering on YbFe 6 ⁢Ge 6 , where the Fe moments in the 2D kagome layers exhibit an 𝐴-type collinear antiferromagnetic order below 𝑇 N ≈ 500 K. Interactions between the Fe ions in the layers and the localized Yb magnetic ions in between reorient the 𝑐-axis-aligned Fe moments to the kagome plane below 𝑇 SR ≈ 63 K. Our magnetotransport measurements show an intriguing anomalous Hall effect (AHE) that emerges in the spin-reorientated collinear state, accompanied by the closing of the spin anisotropy gap as revealed from inelastic neutron scattering. The gapless spin excitations and the Yb-Fe interaction are able to support a dynamic scalar spin chirality, which explains the observed AHE. Therefore, our Letter demonstrates that spin fluctuations may provide an additional scattering channel for the conduction electrons and give rise to AHE even in a collinear antiferromagnet.

Yao, Weiliang [Rice Univ., Houston, TX (United Sta↗

Tuning magnetic order in the van der Waals metal $Fe_5GeTe_2$ by cobalt substitution

Fe 5 - x GeTe 2 is a van der Waals material with one of the highest reported bulk Curie temperatures, T C ≈ 310 K . Here, theoretical calculations and experiments are utilized to demonstrate that the magnetic ground state is highly sensitive to local atomic arrangements and the interlayer stacking. Cobalt substitution is found to be an effective way to manipulate the magnetic properties while also increasing the ordering temperature. In particular, cobalt substitution up to ≈ 30 % enhances T C and changes the magnetic anisotropy, while ≈ 50 % cobalt substitution yields an antiferromagnetic state. Single crystal x-ray diffraction evidences a structural change upon increasing the cobalt concentration, with a rhombohedral cell observed in the parent material and a primitive cell observed for ≈ 46 % cobalt content relative to iron. First-principles calculations demonstrate that it is a combination of high cobalt content and the concomitant change to primitive layer stacking that produces antiferromagnetic order. These results illustrate the sensitivity of magnetism in Fe 5 - x GeTe 2 to composition and structure, and emphasize the important role of local structural order-disorder and layer stacking in cleavable magnetic materials.

36 MATERIALS SCIENCE↗