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At least 19 records

Metastable states in the frustrated triangular compounds Ca 3 Co 2 - x Mn x O 6 and Ca 3 Co 2 O 6

The observation of unusual metastable behavior in Ca 3 Co 2 O 6 remains an ongoing puzzle. When the magnetic field is increased at certain very slow rates, evenly spaced steps occur in the magnetization and other physical quantities as a function of magnetic field every 1.2 T. The ground state without steps is approached by slow relaxation processes over hours to days. It is a striking example of extremely slow dynamics arising from geometrical frustration in an otherwise clean and long-range ordered system, and its precise description remains controversial. Here we shed light on the mystery by reporting similar behavior in isostructural Ca 3 Co 2-x MnxO 6 , albeit at magnetic field sweep rates that are six orders of magnitude faster than that in Ca 3 Co 2 O 6 . We observe these steps not only in the magnetization, but also in the magnetostriction, electric polarization, and magnetocaloric effect. Here, we present a study of metastable behavior in both compounds across seven orders of magnitude of magnetic field sweep rates using unique magnets at the National High Magnetic Field Laboratory. The metastable steps occur for intermediate ranges of magnetic field sweep rates, vanishing or evolving for the fastest and slowest sweep rates. Our data support that these metastable steps are an intrinsic feature of the three-dimensionally frustrated geometry of Ising spins in this structural family and thus narrow the number of applicable models.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Magnetoelastic interactions in SrCu 2 (BO 3 ) 2 studied by Raman scattering experiments and first principles calculations

Dynamic and static crystal lattice properties of SrCu 2 (BO 3 ) 2 are studied by means of Raman scattering, magnetostriction, and thermal expansion measurements in magnetic fields to 45 T. Raman experiments versus temperature reveal that some phonon modes show an unusual behavior: their frequencies soften (modes at 200 and 450 cm –1 ) while others harden (modes at 385 and 478 cm –1 ) when decreasing the temperature below 15 K. Magneto-Raman experiments show that their field dependence correlates with their respective temperature dependencies; e.g., modes that are hardened with increasing temperature also harden with applied magnetic fields and modes that become softer with temperature also soften with applied fields. We use density functional theory to successfully model and compute the energies of these modes, classifying them into two types: pantograph (modes that soften when decreasing the temperature) and nonpantograph. We conclude that the former involves the modification of the intradimer exchange interaction J and the latter the interdimer J'. Lastly, dilatometry is used to correlate field-dependent Raman modes to the closing of the spin gap as well as fractional-magnetization stripe states M = 1/4 M s and M = 1/3 M s , where M s is the saturation magnetization.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Fermi-surface topologies and low-temperature phases of the filled skutterudite compounds CeOs 4 Sb 12 and NdOs 4 Sb 12

We use MHz conductivity, torque magnetometer, and magnetization measurements to report on single crystals of CeOs 4 Sb 12 and NdOs 4 Sb 12 using temperatures down to 0.5 K and magnetic fields of up to 60 tesla. The field-orientation dependence of the de Haas-van Alphen and Shubnikov-de Haas oscillations is deduced by rotating the samples about the [ 010 ] and [ 0 $\bar{1}$ 1 1 ] directions. Our results indicate that NdOs 4 Sb 12 has a similar Fermi surface topology to that of the unusual superconductor PrOs 4 Sb 12 , but with significantly smaller effective masses, supporting the importance of local phonon modes in contributing to the low-temperature heat capacity of NdOs 4 Sb 12 . By contrast, CeOs 4 Sb 12 undergoes a field-induced transition from an unusual semimetal into a high-field, high-temperature state characterized by a single, almost spherical Fermi-surface section. Furthermore, the behavior of the phase boundary and comparisons with models of the band structure lead us to propose that the field-induced phase transition in CeOs 4 Sb 12 is similar in origin to the well-known α - γ transition in Ce and its alloys.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

NSF-DMR Highlight from NHMFL-PFF 2017

The alkali-doped fullerides provide the first example of a transition from a three-dimensional Mott insulator to a superconductor, enabling the effects of both dimensionality and electron correlations on superconductivity to be explored. Chemically, the alkali species tunes the superconductivity in the vicinity of the Mott transition by varying the unit cell volume.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Comparing the anomalous Hall effect and the magneto-optical Kerr effect through antiferromagnetic phase transitions in Mn 3 Sn

In the non-collinear antiferromagnet Mn 3 Sn, we compare simultaneous measurements of the anomalous Hall effect (AHE) and the magneto-optical Kerr effect (MOKE) through two magnetic phase transitions: the high-temperature paramagnetic/antiferromagnetic (AF) phase transition at the Néel temperature ( T N ≈ 420 K) and a lower-temperature incommensurate magnetic ordering at T 1 ≈ 270 K. While both the AHE and MOKE are sensitive to the same underlying symmetries of the AF non-collinear spin order, we find that the transition temperatures measured by these two techniques unexpectedly differ by approximately 10 K. Moreover, the applied magnetic field at which the AF order reverses is significantly larger when measured by MOKE than when measured by AHE. Furthermore these results point to a difference between the bulk and surface magnetic properties of Mn 3 Sn.

36 MATERIALS SCIENCE↗

Emptying Dirac valleys in bismuth using high magnetic fields

The Fermi surface of elemental bismuth consists of three small rotationally equivalent electron pockets, offering a valley degree of freedom to charge carriers. A relatively small magnetic field can confine electrons to their lowest Landau level. This is the quantum limit attained in other dilute metals upon application of sufficiently strong magnetic field. Here in this paper we report on the observation of another threshold magnetic field never encountered before in any other solid. Above this field, B empty , one or two valleys become totally empty. Drying up a Fermi sea by magnetic field in the Brillouin zone leads to a manyfold enhancement in electric conductance. We trace the origin of the large drop in magnetoresistance across B empty to transfer of carriers between valleys with highly anisotropic mobilities. The non-interacting picture of electrons with field-dependent mobility explains most results but the Coulomb interaction may play a role in shaping the fine details.

36 MATERIALS SCIENCE↗

Single reconstructed Fermi surface pocket in an underdoped single-layer cuprate superconductor

The observation of a reconstructed Fermi surface via quantum oscillations in hole-doped cuprates opened a path towards identifying broken symmetry states in the pseudogap regime. However, such an identification has remained inconclusive due to the multi-frequency quantum oscillation spectra and complications accounting for bilayer effects in most studies. We overcome these impediments with high-resolution measurements on the structurally simpler cuprate HgBa2CuO4+δ (Hg1201), which features one CuO2 plane per primitive unit cell. We find only a single oscillatory component with no signatures of magnetic breakdown tunnelling to additional orbits. Therefore, the Fermi surface comprises a single quasi-two-dimensional pocket. Quantitative modelling of these results indicates that a biaxial charge density wave within each CuO2 plane is responsible for the reconstruction and rules out criss-crossed charge stripes between layers as a viable alternative in Hg1201. Lastly, we determine that the characteristic gap between reconstructed pockets is a significant fraction of the pseudogap energy

36 MATERIALS SCIENCE↗

Ultra-High Field Magnets for X-Ray and Neutron Scattering using High Temperature Superconductors

X-ray and neutron scattering techniques are capable of acquiring information about the structure and dynamics of quantum matter. However, the high-field magnet systems currently available at x-ray and neutron scattering facilities in the United States are limited to fields of 16 tesla (T) at maximum, which precludes applications that require and/or study ultra-high field states of matter. This gap in capability—and the need to address it—is a central conclusion of the 2005 National Academy of Sciences report by the Committee on Opportunities in High Magnetic Field Science. To address this gap, we propose a magnet development program that would more than double the field range accessible to scattering experiments. With the development and use of new ultra-high field–magnets, the program would bring into view new worlds of quantum matter with profound impacts on our understanding of advanced electronic materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Magnetic-field-induced vortex-lattice transition in HgBa 2 CuO 4 + δ

Measurements of the 17 O nuclear magnetic resonance (NMR) quadrupolar spectrum of apical oxygen in HgBa 2 CuO 4+δ were performed over a range of magnetic fields from 6.4–30 T in the superconducting state. Oxygen-isotope-exchanged single crystals were investigated with doping corresponding to superconducting transition temperatures from 74 K underdoped, to 78 K overdoped. The apical oxygen site was chosen since its NMR spectrum has narrow quadrupolar satellites that are well separated from any other resonance. Nonvortex contributions to the spectra can be deconvolved in the time domain to determine the local magnetic field distribution from the vortices. Numerical analysis using Brandt's Ginzburg-Landau theory was used to find structural parameters of the vortex lattice, penetration depth, and coherence length as a function of magnetic field in the vortex solid phase. From this analysis we report a vortex structural transition near 15 T from an oblique lattice with an opening angle of 73° at low magnetic fields to a triangular lattice with 60° stabilized at high field. The temperature for onset of vortex dynamics has been identified from spin-spin relaxation. This is independent of the magnetic field at sufficiently high magnetic field similar to that reported for YBa 2 Cu 3 O 7 and Bi 2 Sr 2 CaCu 2 O 8+δ and is correlated with mass anisotropy of the material. Here, this behavior is accounted for theoretically only in the limit of very high anisotropy.

36 MATERIALS SCIENCE↗

P13631-E002PF: Pulsed field magnetostriction of Ba 2 CoTeO 6

Ba 2 CoTeO 6 is an insulating material consisting of two magnetic subsystems referred as A and B build of S=1/2 spins. Subsystem A is considered to be a Heisenberg-like antiferromagnet (AFM) on a triangular lattice and subsystem B is a J 1 -J 2 Ising-like AFM on a honey-comb lattice. The magnetic phase transitions are observed at T N1 = 12 K and T N2 =3K for A and B respectively. The application of magnetic fields unveils a rich phase diagram that varies depending on the direction of the applied field for either H ll c or H perp c. To date the phase diagram has been investigated by means of specific heat measurement up to 9T and susceptibility measurements with a SQUID magnetometer up to 7T. Magnetization measured in pulsed magnetic fields up to 60T at 1.3K and 4.2K reveal several steps and plateaux occurring at varying critical fields depending on the crystallographic direction. Common to the magnetization parallel c and perpendicular c is the saturation above 40T.

36 MATERIALS SCIENCE↗

Magnetic ground state of the one-dimensional ferromagnetic chain compounds M (NCS) 2 (thiourea) 2 (M=Ni,Co)

The magnetic properties of the two isostructural molecule-based magnets— Ni ( NCS ) 2 ( thiourea ) 2 , S = 1 [ thiourea = SC ( NH 2 ) 2 ] and Co ( NCS ) 2 ( thiourea ) 2 , S = 3 / 2 —are characterized using several techniques in order to rationalize their relationship with structural parameters and to ascertain magnetic changes caused by substitution of the spin. Zero-field heat capacity and muon-spin relaxation measurements reveal low-temperature long-range ordering in both compounds, in addition to Ising-like ( D < 0 ) single-ion anisotropy ( D Co ~ - 100 K, D Ni ~ - 10 K). Crystal and electronic structure, combined with dc-field magnetometry, affirm highly quasi-one-dimensional behavior, with ferromagnetic intrachain exchange interactions J Co ≈ + 4 K and J Ni ~ + 100 K and weak antiferromagnetic interchain exchange, on the order of J ' ~ - 0.1 K. Furthermore, electron charge- and spin-density mapping reveals through-space exchange as a mechanism to explain the large discrepancy in J -values despite, from a structural perspective, the highly similar exchange pathways in both materials. Both species can be compared to the similar compounds M Cl 2 ( thiourea ) 4 , M = Ni(II) (DTN) and Co(II) (DTC), where DTN is known to harbor two magnetic-field-induced quantum critical points. Direct comparison of DTN and DTC with the compounds studied here shows that substituting the halide Cl - ion for the NCS - ion results in a dramatic change in both the structural and magnetic properties.

36 MATERIALS SCIENCE↗

Magnetic field-temperature phase diagram of multiferroic (NH4)2FeCl5·H2O

Abstract Owing to their overall low energy scales, flexible molecular architectures, and ease of chemical substitution, molecule-based multiferroics are extraordinarily responsive to external stimuli and exhibit remarkably rich phase diagrams. Even so, the stability and microscopic properties of various magnetic states in close proximity to quantum critical points are highly under-explored in these materials. Inspired by these opportunities, we combined pulsed-field magnetization, first-principles calculations, and numerical simulations to reveal the magnetic field–temperature ( B – T ) phase diagram of multiferroic (NH 4 ) 2 FeCl 5 ⋅H 2 O. In this system, a network of intermolecular hydrogen and halogen bonds creates a competing set of exchange interactions that generates additional structure in the phase diagram—both in the vicinity of the spin flop and near the 30 T transition to the fully saturated state. Consequently, the phase diagrams of (NH 4 ) 2 FeCl 5 ⋅H 2 O and its deuterated analog are much more complex than those of other molecule-based multiferroics. The entire series of coupled electric and magnetic transitions can be accessed with a powered magnet, opening the door to exploration and control of properties in this and related materials.

36 MATERIALS SCIENCE↗

Determining single-ion and spatial exchange anisotropies by pulsed-field magnetometry

The magnetic ground-state of the Q1D S = 1 antiferromagnetic (AFM) chain is sensitive to the single-ion anisotropy (D) and the relative strength of intra- (J) and interchain (J’) exchange interactions. The ratios D/J and J’/J dictate the material’s placement on the phase diagram for which three competing phases are known to theoretically exist: Haldane, XY and quantum paramagnetic. We identified [Ni(HF 2 )(pyz) 2 ]SbF 6 (pyz = pyrazine) as a candidate in which to explore proximity to these phases.

36 MATERIALS SCIENCE↗

Resonant torsion magnetometry in anisotropic quantum materials

Unusual behavior in quantum materials commonly arises from their effective low-dimensional physics, reflecting the underlying anisotropy in the spin and charge degrees of freedom. Here we introduce the magnetotropic coefficient k = ∂ 2 F/∂θ 2 , the second derivative of the free energy F with respect to the magnetic field orientation θ in the crystal. We show that the magnetotropic coefficient can be quantitatively determined from a shift in the resonant frequency of a commercially available atomic force microscopy cantilever under magnetic field. This detection method enables part per 100 million sensitivity and the ability to measure magnetic anisotropy in nanogram-scale samples, as demonstrated on the Weyl semimetal NbP. Measurement of the magnetotropic coefficient in the spin-liquid candidate RuCl 3 highlights its sensitivity to anisotropic phase transitions and allows a quantitative comparison to other thermodynamic coefficients via the Ehrenfest relations.

36 MATERIALS SCIENCE↗

Magnetization dynamics and frustration in the multiferroic double perovskite Lu 2 MnCoO 6

Here, we investigate the magnetic ordering and the magnetization dynamics (from kHz to THz time scales) of the double perovskite Lu 2 MnCoO 6 using elastic neutron diffraction, muon spin relaxation, and micro-Hall magnetization measurements. This compound is known to be a type II multiferroic with the interesting feature that a ferromagneticlike magnetization hysteresis loop couples to an equally hysteretic electric polarization in the bulk of the material despite a zero-field magnetic ordering of the type ↑↑↓↓ along Co-Mn spin chains. Here we explore the unusual dynamics of this compound and find extremely strong fluctuations, consistent with the axial next-nearest-neighbor Ising (ANNNI) model for frustrated spin chains. We identify three temperature scales in Lu 2 MnCoO 6 corresponding to the onset of highly fluctuating long-range order below T N = 50±3 K identified from neutron scattering, the onset of magnetic and electric hysteresis, with change in kHz magnetic and electric dynamics below a 30 K temperature scale, and partial freezing of ~MHz spin fluctuations in the muon spin relaxation data below 12 ± 3 K. Our results provide a framework for understanding the multiferroic behavior of this compound and its hysteresis and dynamics.

36 MATERIALS SCIENCE↗

Field-tunable toroidal moment in a chiral-lattice magnet

Abstract Ferrotoroidal order, which represents a spontaneous arrangement of toroidal moments, has recently been found in a few linear magnetoelectric materials. However, tuning toroidal moments in these materials is challenging. Here, we report switching between ferritoroidal and ferrotoroidal phases by a small magnetic field, in a chiral triangular-lattice magnet BaCoSiO 4 with tri-spin vortices. Upon applying a magnetic field, we observe multi-stair metamagnetic transitions, characterized by equidistant steps in the net magnetic and toroidal moments. This highly unusual ferri-ferroic order appears to come as a result of an unusual hierarchy of frustrated isotropic exchange couplings revealed by first principle calculations, and the antisymmetric exchange interactions driven by the structural chirality. In contrast to the previously known toroidal materials identified via a linear magnetoelectric effect, BaCoSiO 4 is a qualitatively new multiferroic with an unusual coupling between several different orders, and opens up new avenues for realizing easily tunable toroidal orders.

36 MATERIALS SCIENCE↗

Magnetic breakdown and spin-zero effect in quantum oscillations in kagome metal CsV3Sb5

Abstract In the recently discovered kagome metal CsV 3 Sb 5 , an intriguing proposal invoking a doped Chern insulator state suggests the presence of small Chern Fermi pockets hosting spontaneous orbital-currents and large orbital magnetic moments. While the net thermodynamic magnetization is nearly insensitive to these moments, due to their antiferromagnetic alignment, their presence can be revealed by the Zeeman effect, which shifts electron energies in magnetic fields with a proportionality given by the effective g −factor. Here, we determine the g -factor using the spin-zero effect in magnetic quantum oscillations. A large g -factor enhancement is visible only in magnetic breakdown orbits between conventional and concentrated Berry curvature Fermi pockets that host large orbital moments. Such Berry-curvature-generated large orbital moments are almost always concealed by other effects. In this system, however, magnetic breakdown orbits due to the proximity to a conventional Fermi-surface section allow them to be visibly manifested in magnetic quantum oscillations. Our results provide a remarkable example of the interplay between electronic correlations and more conventional electronic bands in quantum materials.

36 MATERIALS SCIENCE↗

Quantum oscillations of electrical resistivity in an insulator

In metals, orbital motions of conduction electrons on the Fermi surface are quantized in magnetic fields, which is manifested by quantum oscillations in electrical resistivity. This Landau quantization is generally absent in insulators. Here, we report a notable exception in an insulator—ytterbium dodecaboride (YbB 12 ). The resistivity of YbB 12 , which is of a much larger magnitude than the resistivity in metals, exhibits distinct quantum oscillations. These unconventional oscillations arise from the insulating bulk, even though the temperature dependence of the oscillation amplitude follows the conventional Fermi liquid theory of metals with a large effective mass. Quantum oscillations in the magnetic torque are also observed, albeit with a lighter effective mass.

36 MATERIALS SCIENCE↗