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Register a new userHigh-temperature spin relaxation process in Dy$_2$Ti$_2$O$_7$ probed by $^{47}$Ti-NQR
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We have performed nuclear quadrupole resonance (NQR) experiments on $^{47}$Ti nuclei in Dy$_2$Ti$_2$O$_7$ in the temperature range 70 -- 300 K in order to investigate the dynamics of $4f$ electrons with strong Ising anisotropy. A significant change of the NQR frequency with temperature was attributed to the variation of the quadrupole moment of Dy $4f$ electrons. A quantitative account was given by the mean field analysis of the quadrupole-quadrupole (Q-Q) interaction in the presence of the crystalline-electric-field splitting. The magnitude and the temperature dependence of the nuclear spin-lattice relaxation rate was analyzed, including both the spin-spin and the Q-Q interactions. The results indicate that these two types of interaction contribute almost equally to the fluctuation of Dy magnetic moments.
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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.
Complex behavior poses challenges in extracting models from experiment. An example is spin liquid formation in frustrated magnets like Dy$_2$Ti$_2$O$_7$. Understanding has been hindered by issues including disorder, glass formation, and interpretation of scattering data. Here, we use a novel automated capability to extract model Hamiltonians from data, and to identify different magnetic regimes. This involves training an autoencoder to learn a compressed representation of three-dimensional diffuse scattering, over a wide range of spin Hamiltonians. The autoencoder finds optimal matches according to scattering and heat capacity data and provides confidence intervals. Validation tests indicate that our optimal Hamiltonian accurately predicts temperature and field dependence of both magnetic structure and magnetization, as well as glass formation and irreversibility in Dy$_2$Ti$_2$O$_7$. The autoencoder can also categorize different magnetic behaviors and eliminate background noise and artifacts in raw data. Our methodology is readily applicable to other materials and types of scattering problems.
Determining the fate of the Pauling entropy in the classical spin ice material Dy$_2$Ti$_2$O$_7$ with respect to the third law of thermodynamics has become an important test case for understanding the existence and stability of ice-rule states in general. The standard model of spin ice - the dipolar spin ice model - predicts an ordering transition at $Tapprox 0.15$ K, but recent experiments by Pomaranski $et al.$ suggest an entropy recovery over long time scales at temperatures as high as $0.5$ K, much too high to be compatible with theory. Using neutron scattering and specific heat measurements at low temperatures and with long time scales ($0.35$ K$/10^6$ s and $0.5$ K$/10^5$ s respectively) on several isotopically enriched samples we find no evidence of a reduction of ice-rule correlations or spin entropy. High-resolution simulations of the neutron structure factor show that the spin correlations remain well described by the dipolar spin ice model at all temperatures. Further, by careful consideration of hyperfine contributions, we conclude that the original entropy measurements of Ramirez $et al.$ are, after all, essentially correct: the short-time relaxation method used in that study gives a reasonably accurate estimate of the equilibrium spin ice entropy due to a cancellation of contributions.
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.
We report a study of the thermal conductivity $kappa$ of the spin-ice material Dy$_2$Ti$_2$O$_7$. From the anisotropic magnetic-field dependence of kappa$ and by additional measurements on the phononic reference compounds Y$_2$Ti$_2$O$_7$ and DyYTi$_2$O$_7$, we are able to separate the phononic and the magnetic contributions to the total heat transport, i.e. $kappa_{ph}$ and $kappa_{mag}$, respectively, which both depend on the magnetic field. The field dependent $kappa_{ph}$ arises from lattice distortions due to magnetic-field induced torques on the non-collinear magnetic moments of the Dy ions. For $kappa_{mag}$, we observe a highly anisotropic magnetic-field dependence, which correlates with the corresponding magnetization data reflecting the different magnetic-field induced spin-ice ground states. The magnitude of $kappa_{mag}$ increases with the degree of the ground-state degeneracy. This anisotropic field dependence as well as various hysteresis effects suggest that $kappa_{mag}$ is essentially determined by the mobility of the magnetic monopole excitations in spin ice.
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