Long-range magnetic order in the 5d(2) double perovskite Ba2CaOsO6: comparison with spin-disordered Ba2YReO6.

The B-site ordered double perovskite Ba2CaOsO6 was studied by dc magnetic susceptibility, powder neutron diffraction and muon spin relaxation methods. The lattice parameter is a = 8.3619(6) Å at 280 K and cubic symmetry [Formula: see text] is retained to 3.5 K with a = 8.3462(7) Å. Curie-Weiss susceptibility behaviour is observed for T > 100 K and the derived constants are C = 0.3361(3) emu K mol(-1) and ΘCW = -156.2(3) K, in excellent agreement with literature values. This Curie constant is much smaller than the spin-only value of 1.00 emu K mol(-1) for a 5d(2) Os(6+) configuration, indicating a major influence of spin-orbit coupling. Previous studies had detected both susceptibility and heat capacity anomalies near 50 K but no definitive conclusion was drawn concerning the nature of the ground state. While no ordered Os moment could be detected by powder neutron diffraction, muon spin relaxation (µSR) data show clear long-lived oscillations indicative of a continuous transition to long-range magnetic order below TC = 50 K. An estimate of the ordered moment on Os(6+) is ∼ 0.2 µB, based upon a comparison with µSR data for Ba2YRuO6 with a known ordered moment of 2.2 µB. These results are compared with those for isostructural Ba2YReO6 which contains Re(5+), also 5d(2), and has a nearly identical unit cell constant, a = 8.36278(2) Å-a structural doppelgänger. In contrast, Ba2YReO6 shows ΘCW = - 616 K, and a complex spin-disordered and, ultimately, spin-frozen ground state below 50 K, indicating a much higher level of geometric frustration than in Ba2CaOsO6. The results on these 5d(2) systems are compared to recent theory, which predicts a variety of ferromagnetic and antiferromagnetic ground states. In the case of Ba2CaOsO6, our data indicate that a complex four-sublattice magnetic structure is likely. This is in contrast to the spin-disordered ground state in Ba2YReO6, despite a lack of evidence for structural disorder, for which theory currently provides no clear explanation.

New magnetic phase diagram of (Sr,Ca)2RuO4.

High-T(c) cuprates, iron pnictides, organic BEDT and TMTSF, alkali-doped C(60), and heavy-fermion systems have superconducting states adjacent to competing states exhibiting static antiferromagnetic or spin density wave order. This feature has promoted pictures for their superconducting pairing mediated by spin fluctuations. Sr(2)RuO(4) is another unconventional superconductor which almost certainly has a p-wave pairing. The absence of known signatures of static magnetism in the Sr-rich side of the (Ca, Sr) substitution space, however, has led to a prevailing view that the superconducting state in Sr(2)RuO(4) emerges from a surrounding Fermi-liquid metallic state. Using muon spin relaxation and magnetic susceptibility measurements, we demonstrate here that (Sr,Ca)(2)RuO(4) has a ground state with static magnetic order over nearly the entire range of (Ca, Sr) substitution, with spin-glass behaviour in Sr(1.5)Ca(0.5)RuO(4) and Ca(1.5)Sr(0.5)RuO(4). The resulting new magnetic phase diagram establishes the proximity of superconductivity in Sr(2)RuO(4) to competing static magnetic order.

Neutron Laue diffraction study on the magnetic phase diagram of multiferroic MnWO4 under pulsed high magnetic fields.

We have combined time-of-flight neutron Laue diffraction and pulsed high magnetic fields at the Spallation Neutron Source to study the phase diagram of the multiferroic material MnWO(4). The control of the field-pulse timing enabled an exploration of magnetic Bragg scattering through the time dependence of both the neutron wavelength and the pulsed magnetic field. This allowed us to observe several magnetic Bragg peaks in different field-induced phases of MnWO(4) with a single instrument configuration. These phases were not previously amenable to neutron diffraction studies due to the large fields involved.

Study of the ground state properties of LiHo(x)Y(1-x)F4 using muon spin relaxation.

LiHo(x)Y(1-x)F4 is an insulator where the magnetic Ho3+ ions have an Ising character and interact mainly through magnetic dipolar fields. We used the muon spin relaxation technique to study the nature of its ground state for samples with x ≤ 0.25. In contrast with some previous works, we did not find canonical spin glass behavior down to ≈ 15 mK. Instead, below ≈300 mK we observed temperature-independent dynamic magnetism characterized by a single correlation time. The 300 mK energy scale corresponds to the Ho3+ hyperfine interaction strength, suggesting that this interaction may be involved in the dynamic behavior of the system.

Spatially homogeneous ferromagnetism of (Ga, Mn)As.

Mn-doped GaAs is a ferromagnetic semiconductor, widely studied because of its possible application for spin-sensitive 'spintronics' devices. The material also attracts great interest in fundamental research regarding its evolution from a paramagnetic insulator to a ferromagnetic metal. The high sensitivity of its physical properties to preparation conditions and heat treatments and the strong doping and temperature dependencies of the magnetic anisotropy have generated a view in the research community that ferromagnetism in (Ga, Mn)As may be associated with unavoidable and intrinsic strong spatial inhomogeneity. Muon spin relaxation (muSR) probes magnetism, yielding unique information about the volume fraction of regions having static magnetic order, as well as the size and distribution of the ordered moments. By combining low-energy muSR, conductivity and a.c. and d.c. magnetization results obtained on high-quality thin-film specimens, we demonstrate here that (Ga, Mn)As shows a sharp onset of ferromagnetic order, developing homogeneously in the full volume fraction, in both insulating and metallic films. Smooth evolution of the ordered moment size across the insulator-metal phase boundary indicates strong ferromagnetic coupling between Mn moments that exists before the emergence of fully itinerant hole carriers.

Static magnetic order and superfluid density of RFeAs(O,F) (R=La,Nd,Ce) and LaFePO studied by muon spin relaxation: unusual similarities with the behavior of cuprate superconductors.

Muon spin relaxation measurements in iron-oxypnictide systems have revealed: (1) commensurate long-range order in undoped LaFeAsO; (2) a Bessel function line shape in LaFeAs(O0.97F0.03) which indicates possible incommensurate or stripe magnetism; (3) anomalous weak magnetism existing in superconducting LaFePO, CeFeAs(O0.084F0.16), and NdFeAs(O0.88F0.12) but absent in superconducting LaFeAs(O0.92F0.08); and (4) scaling of the superfluid density with T_{c} in the Ce-, La-, and Nd-FeAs superconductors following a nearly linear relationship found in cuprates.

Absence of broken time-reversal symmetry in the pseudogap state of the high temperature La(2-x)SrxCuO4 superconductor from muon-spin-relaxation measurements.

We have performed zero-field muon-spin-relaxation measurements on single crystals of La(2-x)SrxCuO4 to search for spontaneous currents in the pseudogap state. By comparing measurements on materials across the phase diagram, we put strict upper limits on any possible time-reversal symmetry breaking fields that could be associated with the pseudogap. Comparison between experimental limits and the proposed circulating current states effectively eliminates the possibility that such states exist in this family of materials.