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Register a new userLarge Low Temperature Specific Heat in Pyrochlore Bi$_2$Ti$_2$O$_7$
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Both amorphous and crystalline materials frequently exhibit low temperature specific heats in excess of what is predicted using the Debye model. The signature of this excess specific heat is a peak observed in $C/T^3$ textit{versus} $T$. To understand the curious absence of long-range ordering of local distortions in the crystal structure of pyrochlore Bi$_2$Ti$_2$O$_7$, we have measured the specific heat of crystalline Bi$_2$Ti$_2$O$_7$ and related compounds. We find that the peak in $C/T^3$ versus $T$ in Bi$_2$Ti$_2$O$_7$ falls at a substantially lower temperature than other similar compounds, consistent with the presence of disorder. This thermodynamic evidence for disorder in crystalline Bi$_2$Ti$_2$O$_7$ is consistent with quenched configurational disorder among Bi lone pairs produced by geometrical frustration, which could represent a possible realization of charge ice.
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The oxide pyrochlore Bi$_2$Ti$_2$O$_7$ is in some ways analogous to perovskite PbTiO$_3$, in that Bi$_2$Ti$_2$O$_7$ has two cations, Bi$^{3+}$ and Ti$^{4+}$ in oxidation states that are normally associated with a propensity to off-center. However, unlike PbTiO$_3$, Bi$_2$Ti$_2$O$_7$ is experimentally observed to remain cubic down to 2 K, while the only observed ionic displacements are local and incoherent. Here we report first-principles calculations of the zone-center phonons of the ordered cubic pyrochlore which reveal several lattice instabilities. An analysis of the structural energetics suggest that the ordered cubic pyrochlore is unstable with respect to distortion towards a ferroelectric ground state with a large polarization. Our results suggest a key role of a frustrated soft polar mode in the dielectric properties of bismuth pyrochlores.
By means of ac magnetic-susceptibility measurements, we find evidence for a new magnetic phase of Tb$_2$Ti$_2$O$_7$ below about 140 mK in zero magnetic field. In magnetic fields parallel to [111], this phase---exhibiting frequency- and amplitude-dependent susceptibility and an extremely slow spin dynamics---extends to about 70 mT, at which it gives way to another phase. The field dependence of the susceptibility of this second phase, which extends to about 0.6 T, indicates the presence of a weak magnetization plateau below 50 mK, as has been predicted by a single-tetrahedron four-spin model, giving support to the underlying proposal that the disordered low-field ground state of Tb$_2$Ti$_2$O$_7$ is a quantum spin ice.
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.
Terbium titanate (Tb$_2$Ti$_2$O$_7$) is a spin-ice material with remarkable magneto-optical properties. It has a high Verdet constant and is a promising substrate crystal for the epitaxy of quantum materials with the pyrochlore structure. Large single crystals with adequate quality of Tb$_2$Ti$_2$O$_7$ or any pyrochlore are not available so far. Here we report the growth of high-quality bulk crystals using the Czochralski method to pull crystals from the melt. Prior work using the automated Czochralski method has suffered from growth instabilities like diameter fluctuation, foot formation and subsequent spiraling shortly after the seeding stage. In this study, the volumes of the crystals were strongly increased to several cubic centimeters by means of manual growth control, leading to crystal diameters up to 40 mm and crystal lengths up to 10 mm. Rocking curve measurements revealed full width at half maximum values between 28 and 40 for 222 reflections. The specific heat capacity c$_p$ was measured between room temperature and 1573 K by dynamic differential scanning calorimetry and shows the typical slow parabolic rise. In contrast, the thermal conductivity kappa(T) shows a minimum near 700 K and increases at higher temperature T. Optical spectroscopy was performed at room temperature from the ultraviolet to the near infrared region, and additionally in the near infrared region up to 1623 K. The optical transmission properties and the crystal color are interpreted to be influenced by partial oxidation of Tb$^{3+}$ to Tb$^{4+}$.
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.
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