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At least 883 records · Page 49
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DOE OSTI2020

Ferrimagnetic 120 ° magnetic structure in Cu 2 OSO 4

We report magnetic properties of a 3d 9 (Cu 2+ ) magnetic insulator Cu 2 OSO 4 measured on both powder and single crystal. The magnetic atoms of this compound form layers whose geometry can be described either as a system of chains coupled through dimers or as a kagome lattice where every third spin is replaced by a dimer. Specific heat and DC susceptibility show a magnetic transition at 20 K, which is also confirmed by neutron scattering. Magnetic entropy extracted from the specific heat data is consistent with an S=1/2 degree of freedom per Cu 2+ , and so is the effective moment extracted from DC susceptibility. The ground state has been identified by means of neutron diffraction on both powder and single crystal and corresponds to an ~120° spin structure in which ferromagnetic intradimer alignment results in a net ferrimagnetic moment. No evidence is found for a change in lattice symmetry down to 2 K. Finally, our results suggest that Cu 2 OSO 4 represents a type of model lattice with frustrated interactions where interplay between magnetic order, thermal and quantum fluctuations can be explored.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Field-induced topological Hall effect and double-fan spin structure with a $c$-axis component in the metallic kagome antiferromagnetic compound YMn 6 Sn 6

Geometric frustration in the kagome lattice makes it a great host for the flat electronic band, nontrivial topological properties, and novel magnetism. In this work, we use magnetotransport measurements to map out the field-temperature phase diagram of the centrosymmetric YMn 6 Sn 6 with a Mn kagome lattice and show that the system exhibits the topological Hall effect (THE) with an in-plane applied magnetic field around 240 K. In addition, our neutron diffraction results demonstrate that the observed THE cannot arise from a magnetic skyrmion lattice, but instead from an in-plane field-induced double-fan spin structure with c-axis components. This paper provides a platform to understand the influence of a field-induced novel magnetic structure on magnetoelectric response in topological kagome metals.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Nature of the magnetic stripes in fully oxygenated La 2 CuO 4+y

We present triple-axis neutron scattering studies of static and dynamic magnetic stripes in an optimally oxygen-doped cuprate superconductor, La 2 CuO 4+y , which exhibits a clean superconducting transition at T c = 42 K. Polarization analysis reveals that the magnetic stripe structure is equally represented along both of the tetragonal crystal axes and that the fluctuating stripes display significant weight for in-plane as well as out-of-plane spin components. Both static magnetic order as well as low-energy fluctuations are fully developed in zero applied magnetic field and the low-energy spin fluctuations at ℏω = 0.3 – 10 meV intensify on cooling. We interpret this as an indication that superconductivity and low-energy spin fluctuations coexist microscopically in spatial regions which are separated from domains with static magnetic order.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Flat-band-induced itinerant ferromagnetism in RbCo 2 Se 2

ACo 2 Se 2 (A=K,Rb,Cs) is a homologue of the iron-based superconductor, AFe 2 Se 2 . From a comprehensive study of RbCo 2 Se 2 via measurements of magnetization, transport, neutron diffraction, angle-resolved photoemission spectroscopy, and first-principle calculations, we identify a ferromagnetic order accompanied by an orbital-dependent spin-splitting of the electronic dispersions. However, we identify the ordered moment to be dominated by a d x 2 –y 2 flatband near the Fermi level, which exhibits the largest spin splitting across the ferromagnetic transition, suggesting an itinerant origin of the ferromagnetism. In the broader context of the iron-based superconductors, we find this d x 2 –y 2 flatband to be a common feature in the band structures of both iron chalcogenides and iron pnictides, accessible via heavy electron doping.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Evolution of magnetic field induced ordering in the layered quantum Heisenberg triangular-lattice antiferromagnet Ba 3 CoSb 2 O 9

Quantum fluctuations in the effective spin-12 layered triangular-lattice quantum Heisenberg antiferromagnet Ba 3 CoSb 2 O 9 lift the classical degeneracy of the antiferromagnetic ground state in magnetic field, producing a series of novel spin structures for magnetic fields applied within the crystallographic ab plane, including a celebrated collinear “up-up-down” spin ordering with magnetization equal to 1/3 of the saturation magnetization over an extended field range. Theoretically unresolved, however, are the effects of interlayer antiferromagnetic coupling and transverse magnetic fields on the ground states of this system. Additional magnetic field induced phase transitions are theoretically expected and in some cases have been experimentally observed, but details regarding their number, location, and physical character appear inconsistent with the predictions of existing models. Conversely, an absence of experimental measurements as a function of magnetic-field orientation has left other key predictions of these models untested. To address these issues, in this study we have used specific heat, neutron diffraction, thermal conductivity, and magnetic torque measurements to map out the phase diagram as a function of magnetic field intensity and orientation relative to the crystallographic ab plane. For H||ab, we have discovered an additional magnetic field induced phase transition at low temperature and an unexpected tetracritical point in the high-field phase diagram, which coupled with the apparent second-order nature of the phase transitions eliminates several theoretically proposed spin structures for the high-field phases. Our calorimetric measurements as a function of magnetic field orientation are in general agreement with theory for field-orientation angles close to plane parallel (H||a) but diverge at angles near plane perpendicular; a predicted convergence of two phase boundaries at finite angle and a corresponding change in the order of the field induced phase transition are not observed experimentally. Our results emphasize the role of interlayer coupling in selecting and stabilizing field induced phases, provide guidance on the nature of the magnetic order in each phase, and reveal the need for new physics to account for the nature of magnetic ordering in this archetypal two-dimensional spin-12 triangular-lattice quantum Heisenberg antiferromagnet.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Tuning magnetism and band topology through antisite defects in Sb-doped MnBi 4 ⁢Te 7

The fine control of magnetism and electronic structure in a magnetic topological insulator is crucial in order to realize various novel magnetic topological states including axion insulators, magnetic Weyl semimetals, Chern insulators, etc. Through crystal growth, transport, thermodynamic, neutron diffraction measurements, we show that under Sb doping the newly discovered intrinsic antiferromagnetic (AFM) topological insulator MnBi 4 Te 7 evolves from AFM to ferromagnetic (FM) and then ferrimagnetic. We attribute this to the formation of Mn(Bi,Sb) antisites upon doping, which results in additional Mn sublattices that modify the delicate interlayer magnetic interactions and cause the dominant Mn sublattice to go from AFM to FM. We further investigate the effect of antisites on the band topology using the first-principles calculations. Without considering antisites, the series evolves from AFM topological insulator (x=0) to FM axion insulators. In the exaggerated case of 16.7% of periodic antisites, the band topology is modified and a type-I magnetic Weyl semimetal phase can be realized at intermediate dopings. Therefore, this doping series provides a fruitful platform with continuously tunable magnetism and topology for investigating emergent phenomena, including quantum anomalous Hall effect, Fermi arc states, etc.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Beyond magnons in Nd 2 ScNbO 7 : An Ising pyrochlore antiferromagnet with all-in–all-out order and random fields

We report the low-temperature magnetic properties of Nd 3+ pyrochlore Nd 2 ScNbO 7 . Susceptibility and magnetization show an easy-axis moment, and heat capacity reveals a phase transition to long-range order at T N =371(2) mK with a fully recovered ΔS=Rln(2), 53% of it recovered for T>T N . Elastic neutron scattering shows a long-range all-in all-out magnetic order with low-Q diffuse elastic scattering. Inelastic neutron scattering shows a low-energy flat band, indicating a magnetic Hamiltonian similar to Nd 2 Zr 2 O 7 . Nuclear hyperfine excitations measured by ultra-high-resolution neutron backscattering indicate a distribution of static electronic moments below T N , which may be due to B-site disorder influencing Nd crystal electric fields. Analysis of heat-capacity data shows an unexpected T-linear or T 3/2 term which is inconsistent with conventional magnon quasiparticles, but is consistent with fractionalized spinons or gapless local spin excitations. We use legacy data to show similar behavior in Nd 2 Zr 2 O 7 . Comparing local static moments also reveals a suppression of the nuclear Schottky anomaly in temperature, evidencing a fraction of Nd sites with nearly zero static moment, consistent with exchange-disorder-induced random singlet formation. Finally, taken together, these measurements suggest an unusual fluctuating magnetic ground state which mimics a spin liquid, but may not actually be one.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Phase transitions of the ferroelectric (ND 4 ) 2 FeCl 5 ·D 2 O under magnetic field

Due to the strong coupling between magnetism and ferroelectricity, (ND 4 ) 2 FeCl 5 ·D 2 O exhibits several intriguing magnetic and electric phases. In this Letter, we include higher-order onsite anisotropic spin interactions to explain the ferroelectric phase transitions of (ND 4 ) 2 FeCl 5 ·D 2 O in a magnetic field and to produce the large weights of high-order harmonic components in the cycloid structure that are observed from neutron diffraction experiments. Moreover, we predict a new ferroelectric phase sandwiched between the FE II and FE III phases in a magnetic field. Furthermore, by emphasizing the importance of the higher-order spin anisotropic interactions, our work provides a framework to understand multiferroic materials with rich phase diagrams.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Itinerant G-type antiferromagnet SrCr 2 As 2 studied by magnetization, heat capacity, electrical resistivity, and NMR measurements

Here, the physical properties of itinerant antiferromagnetic (AFM) SrCr 2 As 2 with body-centered tetragonal ThCr 2 Si 2 structure were investigated in single crystalline and polycrystalline forms by electrical resistivity ρ, heat capacity C p , magnetic susceptibility χ versus temperature T, and magnetization M versus applied magnetic field H isotherm measurements as well as 75 As and 53 Cr nuclear magnetic resonance (NMR) measurements in the wide temperature range T = 1.6–900 K. From the χ(T) and 75 As NMR measurements, the G-type AFM state below T N = 615(15) K has been determined, consistent with the previous neutron-diffraction measurements. Direct evidence of magnetic ordering of the Cr spins was shown by the observation of the 53 Cr NMR spectrum under H = 0. From the χ( T) measurements on single-crystal SrCr 2 As 2 under the two different magnetic field directions H|| ab and H || c in the AFM state, the Cr ordered moments are shown to align along the c axis in the G-type AFM state. The metallic state is directly evidenced by the ρ, C p , and NMR measurements, and the density of states at the Fermi energy $\mathscr{D}$(E F ) in the AFM state is estimated to be 7.53 states/eV f.u. for both spin directions which is almost twice the bare $\mathscr{D}$(E F ) estimated from first-principles calculations, suggesting an enhancement of the conduction-carrier mass by a factor of two in the AFM state. The $\mathscr{D}$(E F ) is found to be nearly constant below at least 100 K and is independent of H. The ρ(T) is found to show T-linear behavior above T N and exhibits positive curvature below T N where significant loss of spin-disorder scattering upon magnetic ordering is observed. The resistivity anisotropy of the compound remains moderate ρ c /ρ a ~ 9 through most of the magnetically ordered phase but shows a rapid increase below 50 K.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Anisotropy of the magnetic and transport properties of EuZn 2 As 2

Several recent studies have shown that the anisotropy in the magnetic structure of EuCd 2 As 2 plays a significant role in stabilizing the Weyl nodes. Therefore, to investigate the relationship between magnetic anisotropy and Weyl physics, we present a comparative study between EuZn 2 As 2 and EuCd 2 As 2 that are isostructural but with different magnetic anisotropy. We performed structural analysis, electronic transport, and magnetization experiments on millimeter-sized single crystals of EuZn 2 As 2 , and compared the results to those of EuCd 2 As 2 . By combining the first principle calculations and neutron diffraction experiment, we identify the magnetic ground state of EuZn 2 As 2 as A-type antiferromagnetic order with a transition temperature (T_N = 19.6 K) twice that of EuCd 2 As 2 . Like EuCd 2 As 2 , the negative magnetoresistance of EuZn 2 As 2 is observed after suppressing the resistivity peak at T_N with increasing fields. However, the anisotropy in both transport and magnetization are much reduced in EuZn 2 As 2 . The difference could be ascribed to the weaker spin-orbit coupling, more localized d orbitals, and a larger contribution from the Eu s orbitals in the zinc compound, as suggested by the electronic band calculations. The same band structure effect could be also responsible for the observation of a smaller nonlinear anomalous Hall effect in EuZn 2 As 2 compared to EuCd 2 As 2 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

A-type antiferromagnetic order in semiconducting EuMg 2 Sb 2 single crystals

Eu-based Zintl-phase materials EuA 2 Pn 2 (A = Mg, In, Cd, Zn; Pn = Bi, Sb, As, P) have generated significant recent interest owing to the complex interplay of magnetism and band topology. Here, we investigated the crystallographic, magnetic, and electronic properties of the layered Zintlphase single crystals of EuMg 2 Sb 2 with the trigonal CaAl 2 Si 2 crystal structure (space group $P\bar{3}m1$). Electrical resistivity measurements complemented with angle-resolved photoemission spectroscopy (ARPES) studies and density functional theory (DFT) calculations find an activated behavior with intrinsic conductivity at high temperatures indicating a semiconducting electronic ground state with a narrow energy gap of 370 meV. Magnetic susceptibility and zero-field heat capacity measurements indicate that the compound undergoes antiferromagnetic (AFM) ordering at the Néel temperature T N = 8.0(2) K. Here, zero-field neutron-diffraction measurements reveal that the AFM ordering is A-type where the Eu spins (Eu 2+ , S = 7/2) arranged in ab-plane layers are aligned ferromagnetically in the ab plane and the Eu spins in adjacent layers are aligned antiferromagnetically. Eu-moment reorientation within the ab planes in the trigonal AFM domains associated with a very weak inplane magnetic anisotropy is also evident below T N at low fields < 0.05 T. Although isostructural semimetallic EuMg 2 Bi 2 is reported to host Dirac surface states, the observation of narrow-gap semiconducting behavior in EuMg 2 Sb 2 implies a strong role of spin-orbit coupling (SOC) in tuning the electronic states of these materials. Our DFT studies also suggest, besides the SOC, the more electronegative and smaller Sb than Bi shifts the low-lying conduction bands along the Γ-A direction to higher energy, resulting in an indirect bulk band gap between the Γ and M points for EuMg 2 Sb 2 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Interplay of itinerant electrons and Ising moments in a hybrid honeycomb quantum magnet TmNi 3 Al 9

The interplay between itinerant electrons and local magnetic moments in quantum materials brings about rich and fascinating phenomena and stimulates various developments in the theoretical framework. In this work, thermodynamic, electric transport, and neutron diffraction measurements were performed on a newly synthesized honeycomb lattice magnet TmNi 3 Al 9 . Based on the experimental data, a magnetic-field–temperature phase diagram was constructed, exhibiting three essentially different magnetic regions. Below T N =2.97±0.02KTm 3+ , moments order antiferromagnetically in zero field. We found that the Tm 3+ ions form a pseudodoublet ground state with the Ising-like moments lying normal to the two-dimensional honeycomb layers. Application of a magnetic field along the easy axis gradually suppresses the antiferromagnetic order in favor of an induced ferromagnetic state above the critical field B c =0.92±0.05T. In the vicinity of B c , a strong enhancement of the quantum spin fluctuations was observed. The quantum Ising nature of the local moments and the coupling to itinerant electrons are discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Weak itinerant magnetic phases of La 2 Ni 7

La 2 Ni 7 is an intermetallic compound that is thought to have itinerant magnetism with small moment (~0.15 µ B /Ni) ordering below 65 K. A recent study of single crystal samples by Ribeiro et. al. [Phys. Rev. B 105, 014412 (2022)] determined detailed anisotropic H-T phase diagrams and revealed three zero-field magnetic phase transitions at T 1 ~61.0 K, T 2 ~56.5 K, and T 3 ~42 K. In that study only the highest temperature phase is shown to have a clear ferromagnetic component. Here we present a single crystal neutron diffraction study determining the propagation vector and magnetic moment direction of the three magnetically ordered phases, two incommensurate and one commensurate, as a function of temperature. The higher temperature phases have similar, incommensurate propagation vectors, but with different ordered moment directions. At lower temperatures the magnetic order becomes commensurate with magnetic moments along the c direction as part of a first-order magnetic phase transition. In this study, we find that the low-temperature commensurate magnetic order is consistent with a proposal from earlier DFT calculations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Magnetic Structure and Spin Fluctuation in Colossal Magnetoresistance Ferrimagnet Mn 3 Si 2 Te 6

The ferrimagnetic insulator Mn 3 Si 2 Te 6 , which features a Curie temperature T c at 78 K and a delicate yet consequential magnetic frustration, exhibits colossal magnetoresistance (CMR) when the magnetic field is applied along the magnetic hard axis, surprisingly inconsistent with existing precedents [Y. Ni, H. Zhao, Y. Zhang, B. Hu, I. Kimchi, and G. Cao, Phys. Rev. B 103, L161105 (2021)]. This discovery motivates a thorough single-crystal neutron diffraction study in order to gain insights into the magnetic structure and its hidden correlation with the new type of CMR. Here we report a noncollinear magnetic structure below the T c where the moments lie predominantly within the basal plane but tilt toward the c axis by ≈10° at ambient conditions. A substantial magnetic diffuse scattering decays slowly and persists well above the T c . The evolution of the spin correlation lengths agrees well with the electrical resistivity, underscoring the role of spin fluctuation contributing to the magnetoresistivity near the transition. Further, application of magnetic field along the c axis renders a swift occurrence of CMR but only a slow tilting of the magnetic moments toward the c axis. The unparalleled changes indicate a nonconsequential role of magnetic polarization.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Frustrated magnetic cycloidal structure and emergent Potts nematicity in CaMn 2 P 2

We report neutron-diffraction results on single-crystal CaMn 2 P 2 containing corrugated Mn honeycomb layers, and we determine its ground-state magnetic structure. The diffraction patterns consist of prominent (1/6,1/6, L ) reciprocal-lattice unit (r.l.u.; L = integer) magnetic Bragg reflections, whose temperature-dependent intensities are consistent with a first-order antiferromagnetic phase transition at the Néel temperature T N = 70 (1) K. Our analysis of the diffraction patterns reveals an in-plane 6 × 6 magnetic unit cell with ordered spins that in the principal-axis directions rotate by 60°steps between nearest neighbors on each sublattice that forms the honeycomb structure, consistent with the P A c magnetic space group. We find that a few other magnetic subgroup symmetries (P A 2 /c, P C 2/m, P S 1, P C 2, P C m, P S 1) of the paramagnetic $P\bar{3}m11'$ crystal symmetry are consistent with the observed diffraction pattern. We relate our findings to frustrated J 1 -J 2 -J 3 Heisenberg honeycomb antiferromagnets with single-ion anisotropy and the emergence of Potts nematicity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Anisotropic magnetism and electronic structure of trigonal EuAl 2 Ge 2 single crystals

Understanding the interplay between magnetic and electronic degrees of freedom is of profound recent interest in different Eu-based magnetic topological materials. Here, we studied the magnetic and electronic properties of the layered Zintl-phase compound EuAl 2 Ge 2 crystallizing in the trigonal CaAl 2 Si 2 -type structure. We report zero-field neutron diffraction, temperature T - and magnetic-field H-dependent magnetic susceptibility χ(T, H), isothermal magnetization M(T, H), heat capacity C p (T, H), and electrical resistivity ρ(T, H) measurements, together with T-dependent angle-resolved photoemission spectroscopy (ARPES) measurements complemented with first-principle calculations. EuAl 2 Ge 2 undergoes second-order A-type antiferromagnetic (AFM) ordering below T N = 27.5(5) K, with the Eu moments (Eu 2+ , S = 7/2) aligned ferromagnetically in the ab plane while these layers are stacked antiferromagnetically along the c axis. The critical fields at which all moments become parallel to the field are 37.5(5) and 52.5(5) kOe for H ∥ ab and H ∥ c, respectively. The H = 0 magnetic structure consists of trigonal AFM domains associated with ab-plane magnetic anisotropy and a field-induced reorientation of the Eu spins in the domains is also evident at T = 2 K below the critical field H c1 = 2.5(1) kOe. The ρ(T) measurements reveal metallic behavior transforming into a slight resistivity increase on cooling towards T N . A pronounced loss of spin-disorder scattering is observed below T N . The ARPES results show that EuAl 2 Ge 2 is metallic both above and below T N , and the Fermi surface is anisotropic with two hole pockets at the zone center and one small electron pocket at each M point. In the AFM phase, we directly observe folded bands in ARPES due to the doubling of the magnetic unit cell along the c axis with an enhancement of quasiparticle weight due to the complex change in the coupling between the magnetic moments and itinerant electrons on cooling below T N . The observed electronic structure is well reproduced by first-principle calculations, which also predict the presence of nontrivial electronic states near the Fermi level in the AFM phase with Z 2 topological numbers 1;(000)

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Static and dynamical properties of the spin-$\frac{5}{2}$ nearly ideal triangular lattice antiferromagnet $\mathrm{Ba_3}$ $\mathrm{MnSb_2}$ $\mathrm{O_9}$

Here, we study the ground state and spin excitations in Ba 3 MnSb 2 O 9 , an easy-plane S = 5/2 triangular lattice antiferromagnet. By combining single-crystal neutron scattering, electric spin resonance (ESR), and spin wave calculations, we determine the frustrated quasi-two-dimensional spin Hamiltonian parameters describing the material. While the material has a slight monoclinic structural distortion, which could allow for isosceles-triangular exchanges and biaxial anisotropy by symmetry, we observe no deviation from the behavior expected for spin waves in the in-plane $120$° state. Even the easy-plane anisotropy is so small that it can only be detected by ESR in our study. In conjunction with the quasi-two-dimensionality, our study establishes that Ba 3 MnSb 2 O 9 is a nearly ideal triangular lattice antiferromagnet with the quasiclassical spin S = 5/2, which suggests that it has the potential for an experimental study of Z- or Z 2 -vortex excitations.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Tailoring physical properties of crystals through synthetic temperature control: A case study for new polymorphic NbFeT e 2 phases

Growth parameters play a significant role in the crystal quality and physical properties of layered materials. Here we present a case study on a van der Waals magnetic NbFeTe 2 material. Two different types of polymorphic NbFeTe 2 phases, synthesized at different temperatures, display significantly different behaviors in crystal symmetry, electronic structure, electrical transport, and magnetism. While the phase synthesized at low temperature showing behavior consistent with previous reports, the new phase synthesized at high temperature, has completely different physical properties, such as metallic resistivity, long-range ferromagnetic order, anomalous Hall effect, negative magnetoresistance, and distinct electronic structures. Neutron diffraction reveals out-of-plane ferromagnetism below 70 K, consistent with the electrical transport and magnetic susceptibility studies. Finally, our work suggests that simply tuning synthetic parameters in a controlled manner could be an effective route to alter the physical properties of existing materials potentially unlocking new states of matter, or even discovering new materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗