The pyrochlore material $rm Ho_{2}Ti_{2}O_{7}$ has been suggested to show ``spin ice behaviour. We present neutron scattering and specific heat results that establish unambiguously that Ho$_2$Ti$_2$O$_7$ exhibits spin ice correlations at low temperature. Diffuse magnetic neutron scattering from Ho$_2$Ti$_2$O$_7$ is found to be quite well described by a near neighbour spin ice model and very accurately described by a dipolar spin ice model. The heat capacity is well accounted for by the sum of a dipolar spin ice contribution and an expected nuclear spin contribution, known to exist in other Ho$^{3+}$ salts. These results settle the question of the nature of the low temperature spin correlations in $rm Ho_{2}Ti_{2}O_{7}$ for which contradictory claims have been made.
When degenerate states are separated by large energy barriers, the approach to thermal equilibrium can be slow enough that physical properties are defined by the thermalization process rather than the equilibrium. The exploration of thermalization pushes experimental boundaries and provides refreshing insights into atomic scale correlations and processes that impact steady state dynamics and prospects for realizing solid state quantum entanglement. We present a comprehensive study of magnetic relaxation in Ho$_2$Ti$_2$O$_7$ based on frequency-dependent susceptibility measurements and neutron diffraction studies of the real-time atomic-scale response to field quenches. Covering nearly ten decades in time scales, these experiments uncover two distinct relaxation processes that dominate in different temperature regimes. At low temperatures (0.6K<T<1K) magnetic relaxation is associated with monopole motion along the applied field direction through the spin-ice vacuum. The increase of the relaxation time upon cooling indicates reduced monopole conductivity driven by decreasing monopole concentration and mobility as in a semiconductor. At higher temperatures (1K<T<2K) magnetic relaxation is associated with the reorientation of monopolar bound states as the system approaches the single-spin tunneling regime. Spin fractionalization is thus directly exposed in the relaxation dynamics.
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.
Recent studies on Rb2Ti2O5 crystals have demonstrated remarkable electrical properties. This material exhibits colossal electrical polarization between 200 K and 330 K. In the present work, we report on the observation of memory effects in Rb2Ti2O5 due to charge accumulation and we discuss the genuine memristive character of this material. An analytical model is proposed for the system, which takes into account the ionic diffusion and ionic migration and is in good agreement with the observed volatile memristive properties of the material.
We present an extensive study on the effect of substrate orientation, strain, stoichiometry and defects on spin ice physics in Ho$_2$Ti$_2$O$_7$ thin films grown onto yttria-stabilized-zirconia substrates. We find that growth in different orientations produces different strain states in the films. All films exhibit similar c-axis lattice parameters for their relaxed portions, which are consistently larger than the bulk value of 10.10 AA. Transmission electron microscopy reveals anti-site disorder and growth defects to be present in the films, but stuffing is not observed. The amount of disorder depends on the growth orientation, with the (110) film showing the least. Magnetization measurements at 1.8 K show the expected magnetic anisotropy and saturation magnetization values associated with a spin ice for all orientations; shape anisotropy is apparent when comparing in and out-of-plane directions. Significantly, only the (110) oriented films display the hallmark spin ice plateau state in magnetization, albeit less well-defined compared to the plateau observed in a single crystal. Neutron scattering maps on the more disordered (111) oriented films show the Q=0 phase previously observed in bulk materials, but the Q=X phase giving the plateau state remains elusive. We conclude that the spin ice physics in thin films is modified by defects and strain, leading to a reduction in the temperature at which correlations drive the system into the spin ice state.
The elementary excitations of the spin-ice materials Ho$_2$Ti$_2$O$_7$ and Dy$_2$Ti$_2$O$_7$ in zero field can be described as independent magnetic monopoles. We investigate the influence of these exotic excitations on the heat transport by measuring the magnetic-field dependent thermal conductivity $kappa $. Additional measurements on the highly dilute reference compounds HoYTi$_2$O$_7$ and DyYTi$_2$O$_7$ enable us to separate $kappa $ into a sum of phononic ($kappa_{ph}$) and magnetic ($kappa_{mag}$) contributions. For both spin-ice materials, we derive significant zero-field contributions $kappa_{mag}$, which are rapidly suppressed in finite magnetic fields. Moreover, $kappa_{mag}$ sensitively depends on the scattering of phonons by magnetic excitations, which is rather different for the Ho- and the Dy-based materials and, as a further consequence, the respective magnetic-field dependent changes $kappa_{ph}(B)$ are even of opposite signs.