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We study the stability of the antiferromagnetic all-in--all-out state observed in dipolar-octupolar pyrochlores that have neodymium as the magnetic species. Different types of disorder are considered, either affecting the immediate environment of the Nd$^{3+}$ ion, or substituting it with a non-magnetic ion. Starting from the well studied Nd$_2$Zr$_2$O$_7$ compound, Ti substitution on the Zr site and dilution on the Nd magnetic site with La substitution are investigated. The recently discovered entropy stabilized compound NdMox, which exhibits a high degree of disorder on the non magnetic site is also studied. Using a range of experimental techniques, especially very low-temperature magnetization and neutron scattering, we show that the all-in--all-out state is very robust and withstands substitutional disorder up to large rates. From these measurements, we estimate the Hamiltonian parameters and discuss their evolution in the framework of the phase diagram of dipolar-octupolar pyrochlore magnets., Comment: 19 pages, 20 figures (main text: 12 pages, 13 figures)

We have investigated the origin of the magnetic dipole correlations $\langle \sigma_{\boldsymbol{Q}}^z \sigma_{\boldsymbol{-Q}}^z \rangle$ characterized by the modulation wave vector $\boldsymbol{k} \sim (\tfrac{1}{2},\tfrac{1}{2},\tfrac{1}{2})$ observed in the frustrated pyrochlore magnet Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$. This magnetic short-range order cannot be accounted for by adding further-neighbor exchange interactions to the nearest-neighbor pseudospin-$\tfrac{1}{2}$ Hamiltonian for quantum pyrochlore magnets. Using classical Monte Carlo simulation and quantum simulation based on thermally pure quantum (TPQ) states we have shown that the spin correlations with $\boldsymbol{k} \sim (\tfrac{1}{2},\tfrac{1}{2},\tfrac{1}{2})$ are induced at low temperatures by a three-spin interaction of a form $\sigma_{\boldsymbol{r}}^{\pm} \sigma_{\boldsymbol{r}^{\prime}}^z \sigma_{\boldsymbol{r}^{\prime \prime}}^z $, which is a correction to the Hamiltonian due to the low crystal-field excitation. Simulations using TPQ states have shown that the spin correlations coexist with electric quadrupole correlations $\langle \sigma_{\boldsymbol{Q}}^{\alpha} \sigma_{\boldsymbol{-Q}}^{\beta} \rangle$ ($\alpha, \beta = x, y$) with $\boldsymbol{k} \sim \boldsymbol{0}$. These results suggest that the putative quantum spin liquid state of Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ is located close to phase boundaries of the spin-ice, quadrupole-ordered, and magnetic-ordered states in the classical approximation, and that the three-spin interaction brings about a quantum disordered ground state with both spin and quadrupole correlations., Comment: 28 pages, 25 figures

Magnetic excitations of the recently discovered frustrated spin-1/2 two-leg ladder system Li$_2$Cu$_2$O(SO$_4$)$_2$ are investigated using inelastic neutron scattering, magnetic susceptibility and infrared absorption measurements. Despite the presence of a magnetic dimerization concomitant with the tetragonal-to-triclinic structural distortion occurring below 125 K, neutron scattering experiments reveal the presence of dispersive triplet excitations above a spin gap of $\Delta = 10.6$ meV at 1.5 K, a value consistent with the estimates extracted from magnetic susceptibility. The likely detection of these spin excitations in infrared spectroscopy is explained by invoking a dynamic Dzyaloshinskii-Moriya mechanism in which light is coupled to the dimer singlet-to-triplet transition through an optical phonon. These results are qualitatively explained by exact diagonalization and higher-order perturbation calculations carried out on the basis of the dimerized spin Hamiltonian derived from first-principles., Comment: to appear in Phys. Rev. B, 10 pages including 7 figure (supplemental series provided as ancillary files)

Spin correlations of the frustrated pyrochlore oxide Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ have been investigated by using inelastic neutron scattering on single crystalline samples ($x=-0.007, 0.000,$ and $0.003$), which have the putative quantum-spin-liquid (QSL) or electric-quadrupolar ground states. Spin correlations, which are notably observed in nominally elastic scattering, show short-ranged correlations around $L$ points [$q = (\tfrac{1}{2},\tfrac{1}{2},\tfrac{1}{2})$], tiny antiferromagnetic Bragg scattering at $L$ and $\Gamma$ points, and pinch-point type structures around $\Gamma$ points. The short-ranged spin correlations were analyzed using a random phase approximation (RPA) assuming the paramagnetic state and two-spin interactions among Ising spins. These analyses have shown that the RPA scattering intensity well reproduces the experimental data using temperature and $x$ dependent coupling constants of up to 10-th neighbor site pairs. This suggests that no symmetry breaking occurs in the QSL sample, and that a quantum treatment beyond the semi-classical RPA approach is required. Implications of the experimental data and the RPA analyses are discussed., Comment: 13 pages, 11 figures

The ground states of the frustrated pyrochlore oxide Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ have been studied by inelastic neutron scattering experiments. Three single-crystal samples are investigated; one shows no phase transition ($x=-0.007

Excitations in a spin ice behave as magnetic monopoles, and their population and mobility control the dynamics of a spin ice at low temperature. CdEr$_2$Se$_4$ is reported to have the Pauling entropy characteristic of a spin ice, but its dynamics are three-orders of magnitude faster than the canonical spin ice Dy$_2$Ti$_2$O$_7$. In this letter we use diffuse neutron scattering to show that both CdEr$_2$Se$_4$ and CdEr$_2$S$_4$ support a dipolar spin ice state -- the host phase for a Coulomb gas of emergent magnetic monopoles. These Coulomb gases have similar parameters to that in Dy$_2$Ti$_2$O$_7$, i.e. dilute and uncorrelated, so cannot provide three-orders faster dynamics through a larger monopole population alone. We investigate the monopole dynamics using ac susceptometry and neutron spin echo spectroscopy, and verify the crystal electric field Hamiltonian of the Er$^{3+}$ ions using inelastic neutron scattering. A quantitative calculation of the monopole hopping rate using our Coulomb gas and crystal electric field parameters shows that the fast dynamics in CdEr$_2$X$_4$ (X = Se, S) are primarily due to much faster monopole hopping. Our work suggests that CdEr$_2$X$_4$ offer the possibility to study alternative spin ice ground states and dynamics, with equilibration possible at much lower temperatures than the rare earth pyrochlore examples., Comment: 11 pages, 9 figures, accepted for publication in Physical Review Letters

We report the low temperature magnetic properties of the pyrochlore Pr$_2$Hf$_2$O$_7$. Polycrystalline and single-crystal samples are investigated using time-of-flight neutron spectroscopy and macroscopic measurements, respectively. The crystal-field splitting produces a non-Kramers doublet ground state for Pr$^{3+}$, with Ising-like anisotropy. Below 0.5 K ferromagnetic correlations develop, which suggests that the system enters a spin ice-like state associated with the metamagnetic behavior observed at $\mu_0H_c\sim2.4$~T. In this regime, the development of a discrete inelastic excitation in the neutron spectra indicates the appearance of spin dynamics which are likely related to cooperative quantum fluctuations., Comment: 7 pages, 5 figures, 1 table