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Register a new userExperimental observation of magnetoelectricity in spin ice Dy$_2$Ti$_2$O$_7$
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The intrinsic noncollinear spin patterns in rare-earth pyrochlore are physically interesting, hosting many emergent properties, e.g. spin ice and monopole-type excitation. Recently, the magnetic monopole excitation of spin ice systems was predicted to be magnetoelectric active, while rare experimental works have directly confirmed this scenario. In this work, we performed systematic experimental investigation on the magnetoelectricity of Dy$_2$Ti$_2$O$_7$ by probing the ferroelectricity, spin dynamics, and dielectric behaviors. Two ferroelectric transitions at $T_{c1}$=25 K and $T_{c2}$=13 K have been observed. Remarkable magnetoelectric coupling is identified below the lower transition temperature, with a significant suppression of the electric polarization upon applied magnetic field. It is surprised that the lower ferroelectric transition temperature just coincides with the Ising-spin paramagnetic transition point, below which the quasi-particle-like monopoles are populated, indicating implicit correlation between electric dipoles and spin moments. The possible magnetoelectric mechanisms have also been discussed although a decent theory remains unavailable up to date. Our results will stimulate more investigations to explore multiferroicity in these spin ice systems and other frustrated magnets.
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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.
The Raman spectroscopy and AC and DC magnetization of Dy$_{2-x}$Eu$_x$Ti$_2$O$_7$ have been investigated. In Raman Spectroscopy, the systematic shift in all phonon modes with Eu content in Dy$_{2-x}$Eu$_x$Ti$_2$O$_7$ confirms that Dy$^{3+}$ ion is substituted by Eu3+ ions. High concentration of Eu induces the dipolar exchange interactions and crystal-field interactions in Dy$_{2-x}$Eu$_x$Ti$_2$O$_7$. Rich Eu content samples (x=1.8 and 1.9) show the existence of wasp-waisted hysteresis loop and that can be attributed to the coexistence of dipolar field and anisotropy exchange interaction. AC susceptibility shows two single ion spin freezing transitions corresponding to Dy$^{3+}$ and Eu$^{3+}$ ions respectively in x = 1.5, 1.8, 1.9 samples.
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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