Edwin Kermarrec

The frustrated fcc antiferromagnet Ba2 YOsO6: Structural characterization, magnetic properties and neutron scattering studies

Here we report the crystal structure, magnetization, and neutron scattering measurements on the double perovskite Ba2 YOsO6. The Fm

Low-energy electrodynamics of novel spin excitations in the quantum spin ice Yb 2 Ti 2 O 7

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Ground state selection under pressure in the quantum pyrochlore magnet Yb 2 Ti 2 O 7

m space group is found both at 290 K and 3.5 K with cell constants a0=8.3541(4) A and 8.3435(4) A, respectively. Os5+ (5d3) ions occupy a nondistorted, geometrically frustrated face-centered-cubic (fcc) lattice. A Curie-Weiss temperature θ ~₋700 K suggests the presence of a large antiferromagnetic interaction and a high degree of magnetic frustration. A magnetic transition to long-range antiferromagnetic order, consistent with a type-I fcc state below TN~69 K, is revealed by magnetization, Fisher heat capacity, and elastic neutron scattering, with an ordered moment of 1.65(6) μB on Os5+. The ordered moment is much reduced from either the expected spin-only value of ~3 μB or the value appropriate to 4d3 Ru5+ in isostructural Ba2 YRuO6 of 2.2(1) μB, suggesting a role for spin-orbit coupling (SOC). Triple-axis neutron scattering measurements of the order parameter suggest an additional first-order transition at T=67.45 K, and the existence of a second-ordered state. We find time-of-flight inelastic neutron results reveal a large spin gap Δ~17 meV, unexpected for an orbitally quenched, d3 electronic configuration. In conclusion, we discuss this in the context of the ~5 meV spin gap observed in the related Ru5+,4d3 cubic double perovskite Ba2YRuO6, and attribute the ~3 times larger gap to stronger SOC present in this heavier, 5d, osmate system.

Cubic Re6+ (5d1) Double Perovskites, Ba2MgReO6, Ba2ZnReO6, and Ba2Y2/3ReO6: Magnetism, Heat Capacity, μSR, and Neutron Scattering Studies and Comparison with Theory

Significance Magnetic materials are composed of individual spins that interact with each other and under suitable conditions can arrange themselves in an ordered array. When spins are confined to two-dimensional sheets, small perturbations can disrupt their order and destroy the magnetic state. We show how a set of interacting, quantum-mechanical spins placed on the corners of a square array evolves from a set of locally bonded entities to a globally ordered structure. The system stabilizes itself against fluctuations through subtle local contractions, elongations, and tilts. The combination of neutron and X-ray scattering at pressures up to 60,000 atmospheres reveals the complex interplay of structural distortions and spin alignments that permit long-range order to emerge in this model quantum magnet. Quantum spins placed on the corners of a square lattice can dimerize and form singlets, which then can be transformed into a magnetic state as the interactions between dimers increase beyond threshold. This is a strictly 2D transition in theory, but real-world materials often need the third dimension to stabilize long-range order. We use high pressures to convert sheets of Cu2+ spin 1/2 dimers from local singlets to global antiferromagnet in the model system SrCu2(BO3)2. Single-crystal neutron diffraction measurements at pressures above 5 GPa provide a direct signature of the antiferromagnetic ordered state, whereas high-resolution neutron powder and X-ray diffraction at commensurate pressures reveal a tilting of the Cu spins out of the plane with a critical exponent characteristic of 3D transitions. The addition of anisotropic, interplane, spin–orbit terms in the venerable Shastry–Sutherland Hamiltonian accounts for the influence of the third dimension.

Magnetic dilution and domain selection in the X Y pyrochlore antiferromagnet Er 2 Ti 2 O 7

In condensed matter systems, formation of long-range order (LRO) is often accompanied by new excitations. However, in many geometrically frustrated magnetic systems, conventional LRO is suppressed, while non-trivial spin correlations are still observed. A natural question to ask is then what is the nature of the excitations in this highly correlated state without broken symmetry? Frequently, applying a symmetry breaking field stabilizes excitations whose properties reflect certain aspects of the anomalous state without LRO. Here we report a THz spectroscopy study of novel excitations in quantum spin ice Yb2Ti2O7 under a <001> directed magnetic field. At large positive fields, both right- and left-handed magnon and two-magnon-like excitations are observed. The g-factors of these excitations are dramatically enhanced in the low-field limit, showing a crossover of these states into features consistent with the quantum string-like excitations proposed to exist in quantum spin ice in small <001> fields.

Reply to Zayed: Interplay of magnetism and structure in the Shastry–Sutherland model

We know the ground state of the quantum spin ice candidate magnet Yb2Ti2O7 to be sensitive to weak disorder at the similar to 1% level which occurs in single crystals grown from the melt. Powders produced by solid state synthesis tend to be stoichiometric and display large and sharp heat capacity anomalies at relatively high temperatures, T-C similar to 0.26 K. We have carried out neutron elastic and inelastic measurements on well characterized and equilibrated stoichiometric powder samples of Yb2Ti2O7 which show resolution-limited Bragg peaks to appear at low temperatures, but whose onset correlates with temperatures much higher than T-C. The corresponding magnetic structure is best described as an icelike splayed ferromagnet. In the spin dynamics of Yb2Ti2O7 we see the gapless on an energy scale <0.09 meV at all temperatures and organized into a continuum of scattering with vestiges of highly overdamped ferromagnetic spin waves present. These excitations differ greatly from conventional spin waves predicted for Yb2Ti2O7s mean field ordered state, but appear robust to weak disorder as they are largely consistent with those displayed by nonstoichiometric crushed single crystals and single crystals, as well as by powder samples of Yb2Ti2O7s sister quantum magnet Yb2Ti2O7.

Neutron spectroscopic study of crystalline electric field excitations in stoichiometric and lightly stuffed Yb2Ti2O7

A quantum spin liquid is a state of matter characterized by quantum entanglement and the absence of any broken symmetry. In condensed matter, the frustrated rare-earth pyrochlore magnets Ho2Ti2O7 and Dy2Ti2O7, so-called spin ices, exhibit a classical spin liquid state with fractionalized thermal excitations (magnetic monopoles). Evidence for a quantum spin ice, in which the magnetic monopoles become long range entangled and an emergent quantum electrodynamics arises, seems within reach. The magnetic properties of the quantum spin ice candidate Yb2Ti2O7 have eluded a global understanding and even the presence or absence of static magnetic order at low temperatures is controversial. Here we show that sensitivity to pressure is the missing key to the low temperature behaviour of Yb2Ti2O7. By combining neutron diffraction and muon spin relaxation on a stoichiometric sample under pressure, we evidence a magnetic transition from a disordered, non-magnetic, ground state to a splayed ferromagnetic ground state.

Neutron scattering in

Double perovskites (DP) of the general formula Ba2MReO6, where M = Mg, Zn, and Y2/3, all based on Re6+ (5d1, t2g1), were synthesized and studied using magnetization, heat capacity, muon spin relaxation, and neutron-scattering techniques. All are cubic, Fm3̅m, at ambient temperature to within the resolution of the X-ray and neutron diffraction data, although the muon data suggest the possibility of a local distortion for M = Mg. The M = Mg DP is a ferromagnet, Tc = 18 K, with a saturation moment ∼0.3 bohr magnetons at 3 K. There are two anomalies in the heat capacity: a sharp feature at 18 K and a broad maximum centered near 33 K. The total entropy loss below 45 K is 9.68 e.u., which approaches R ln 4 (11.52 e.u.) supporting a j = 3/2 ground state. The unit cell constants of Ba2MgReO6 and the isostructural, isoelectronic analogue, Ba2LiOsO6, differ by only 0.1%, yet the latter is an anti-ferromagnet. The M = Zn DP also appears to be a ferromagnet, Tc = 11 K, μsat(Re) = 0.1 μB. In this case the heat capacity shows a somewhat broad peak near 10 K and a broader maximum at ∼33 K, behavior that can be traced to a smaller particle size, ∼30 nm, for this sample. For both M = Mg and Zn, the low-temperature magnetic heat capacity follows a T3/2 behavior, consistent with a ferromagnetic spin wave. An attempt to attribute the broad 33 K heat capacity anomalies to a splitting of the j = 3/2 state by a crystal distortion is not supported by inelastic neutron scattering, which shows no transition at the expected energy of ∼7 meV nor any transition up to 100 meV. However, the results for the two ferromagnets are compared to the theory of Chen, Pereira, and Balents, and the computed heat capacity predicts the two maxima observed experimentally. The M = Y2/3 DP, with a significantly larger cell constant (3%) than the ferromagnets, shows predominantly anti-ferromagnetic correlations, and the ground state is complex with a spin frozen component Tg = 16 K from both direct current and alternating current susceptibility and μSR data but with a persistent dynamic component. The low-temperature heat capacity shows a T1 power law. The unit cell constant of B = Y2/3 is less than 1% larger than that of the ferromagnetic Os7+ (5d1) DP, Ba2NaOsO6.