Muons and magnets

Abstract:

Magnetic heat capacity measurements of a high-quality single crystal of the dipole-octupole pyrochlore Ce2Hf2O7 down to a temperature of T=0.02 K are reported. These show a two-peaked structure, with a Schottky-like peak at T1∼0.065 K, similar to what is observed in its sister Ce pyrochlores Ce2Zr2O7 and Ce2Sn2O7. However, a second sharper peak is observed at T2∼0.025 K, signifying the entrance to the ground state. The ground state appears to have gapped excitations, as even the most abrupt extrapolation to CP=0 at T=0 K fully accounts for the Rln(2) entropy associated with the pseudospin-1/2 doublet for Ce3+ in this environment. The ground state could be conventionally ordered, although theory predicts a much larger anomaly in CP at much higher temperatures than the measured T2 for expectations from an all-in, all-out ground state of the XYZ Hamiltonian for Ce2Hf2O7. The sharp low-temperature peak could also signify a crossover from a classical spin liquid to a quantum spin liquid (QSL). For both scenarios, comparison of the measured CP with NLC calculations suggests that weak interactions beyond the nearest-neighbor XYZ Hamiltonian become relevant below T∼0.25 K. The diffuse magnetic neutron scattering observed from Ce2Hf2O7 at low temperatures between T2 and T1 resembles that observed from Ce2Zr2O7, which is well established as a π-flux quantum spin ice (QSI). Together with the peak in the heat capacity at T2, this diffuse scattering from Ce2Hf2O7 is suggestive of a classical spin liquid regime above T2 that is distinct from the zero-entropy quantum ground state below T2.

Abstract:

We present single-crystal neutron diffraction, powder muon spin rotation, and pulsed-field magnetometry measurements on the Heisenberg quantum chiral chain $\left[\mathrm{Cu}\left(\mathrm{pym}\right){\left({\mathrm{H}}_2\mathrm{O}\right)}_4\right]{\mathrm{SiF}}_6·{\mathrm{H}}_2\mathrm{O}$ (pym = pyrimidine), which displays a fourfold-periodic rotation of the local environment around the Cu() $S=1/2$ ions from site to site along the chain. Previous measurements on this material have shown the absence of magnetic order down to surprisingly low temperatures $\ge 20$  mK, as well as the presence of an energy gap for magnetic excitations that grows linearly with magnetic field. Here we find evidence at dilution refrigerator temperatures for a field-induced transition to long-range magnetic order above an applied magnetic field of 3 T. From the polarization of magnetic moments observed with magnetic fields applied in the $[-1,2,0]$ direction, we can identify the static magnetic structure that best accounts for the data. The proposed model is supported microscopically by the presence of an alternating component of the $g$ tensor, which produces an internal twofold staggered field that dictates both the direction of the ordered moments and the effective coupling between adjacent chains. The observed magnetic structure is contrary to previous proposals for the departure of the magnitude and field dependence of the energy gap from the predictions of the sine-Gordon model.

Abstract:

${\text{YbZn}}_2{\mathrm{GaO}}_5$ is a promising candidate for realizing a quantum spin liquid (QSL) state, particularly owing to its lack of significant site disorder. Pulsed-field magnetometry at 0.5 K shows magnetization saturating near 15 T, with a corrected saturation moment of $2.1(1){\mu }_{\mathrm{B}}$ after subtracting the van Vleck contribution. Our zero-field $\mathrm{\mu }\mathrm{SR}$ measurements down to milliKelvin temperatures provide evidence for a dynamic ground state and the absence of magnetic order. To probe fluctuations in the local magnetic field at the muon site, we performed longitudinal field $\mathrm{\mu }\mathrm{SR}$ experiments. These results provide evidence for spin dynamics with a field dependence that is consistent with a U1A01 Dirac quantum spin liquid as a plausible description of the ground state.

Abstract:

Ruddlesden-Popper oxide phases in the LaxSr2−xCo0.5Ir0.5O4 (0 < x < 1) solid solution can be converted to the corresponding LaxSr2−xCo0.5Ir0.5O4−yHy oxyhydride phases, by topochemical reaction with LiH, in which the hydride ions are substituted exclusively onto the equatorial anion sites of the host framework. Analysis reveals that oxyhydride phases in the range 0.5 < x < 1 adopt LaxSr2−xCo0.5Ir0.5O2+xH2−x compositions which maintain a constant Co1+, Ir3+ oxidation-state combination (confirmed by Co K-edge XANES data), with the presence of low-spin d6 Ir3+ being consistent with the covalent stabilization of the metastable oxyhydride phases via strong Ir–H σ-bonds. Phases at the lanthanum-poor end of the solid solution (x < 0.5) adopt LaxSr2−xCo0.5Ir0.5O4−yHy compositions with lower hydride concentrations (y < 1.5). Magnetisation and μSR data indicate that all the LaxSr2−xCo0.5Ir0.5O4−yHy oxyhydride phases exhibit strong magnetic frustration, attributed to the large-scale cation and anion disorder, and resulting in glassy magnetic behaviour at low temperature.

Abstract:

Kagome lattice decorated with S=1/2 spins is one of the most discussed ways to realize a quantum spin liquid. However, all previous material realizations of this model have suffered from additional complications, ranging from additional interactions to impurity effects. Recently, a new quantum kagome system has been identified in the form of averievite Cu5−xZnxV2O10(CsCl), featuring a unique double-layer spacing between the kagome planes. Using muon spin spectroscopy we show that only a complete substitution (i.e., x=2) of interplanar copper ions leads to a quantum-disordered ground state. In contrast, the parent compound (x=0) exhibits long-range magnetic order, with a phase transition around 24 K. Experiments performed on the partially substituted material (x=1) show that the transformation proceeds through an intermediate disordered, partially frozen ground state, unaffected by pressures up to 23 kbar. Our study provides a microscopic view of the magnetism of the decoupling of the kagome layers and establishes the averievite as a new material platform for the experimental study of the fully-decoupled kagome layers.