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Register a new userFar-infrared optical properties of the pyrochlore spin ice compound Dy2Ti2O4
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Near normal incident far-infrared reflectivity spectra of [111] dysprosium titanate (Dy2Ti2O4) single crystal have been measured at different temperatures. Seven phonon modes (eight at low temperature) are identified at frequency below 1000 cm-1. Optical conductivity spectra are obtained by fitting all the reflectivity spectra with the factorized form of the dielectric function. Both the Born effective charges and the static optical primitivity are found to increase with decreasing temperature. Moreover, phonon linewidth narrowering and phonon modes shift with decreasing temperature are also observed, which may result from enhanced charge localization. The redshift of several low frequency modes is attributed to the spin-phonon coupling. All observed optical properties can be explained within the framework of nearest neighbor ferromagnetic(FM) spin ice model.
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We present reflectance measurements in the infrared region on a single crystal the rare earth scandate DyScO3. Measurements performed between room temperature and 10 K allow to determine the frequency of the infrared-active phonons, never investigated experimentally, and to get information on their temperature dependence. A comparison with the phonon peak frequency resulting from ab-initio computations is also provided. We finally report detailed data on the frequency dependence of the complex refractive index of DyScO3 in the terahertz region, which is important in the analysis of terahertz measurements on thin films deposited on DyScO3.
We present here temperature-dependent Raman, x-ray diffraction and specific heat studies between room temperature and 12 K on single crystals of spin-ice pyrochlore compound $Dy_2Ti_2O_7$ and its non-magnetic analogue $Lu_2Ti_2O_7$. Raman data show a new band not predicted by factor group analysis of Raman-active modes for the pyrochlore structure in $Dy_2Ti_2O_7$, appearing below a temperature of $T_c=$110 K with a concomitant contraction of the cubic unit cell volume as determined from the powder x-ray diffraction analysis. Low temperature Raman experiments on O$^{18}$-isotope substituted $Dy_2Ti_2O_7$ confirm the phonon origin of the new mode. These findings, absent in $Lu_2Ti_2O_7$, suggest that the room temperature cubic lattice of the pyrochlore $Dy_2Ti_2O_7$ undergoes a subtle structural transformation near $T_c$. We find anomalous textit{red-shift} of some of the phonon modes in both the $Dy_2Ti_2O_7$ and the $Lu_2Ti_2O_7$ as the temperature decreases, which is attributed to strong phonon-phonon anharmonic interactions.
Pyrochlore $rm Pr^{3+}_{2+x}Zr^{4+}_{2-x}O_{7-x/2}$ samples in the form of both powders $(-0.02 le x le 0.02)$ and bulk single crystals have been studied to elucidate the dependence of their magnetic, compositional and structural properties on synthesis and growth conditions. All samples were characterized using X-ray diffraction, specific heat, and DC magnetization measurements. The crystals were also studied using the X-ray Laue technique and scanning electron microscopy. Increasing the Pr content for the $rm Pr_{2+x}Zr_{2-x}O_{7-x/2}$ powders enlarged the lattice parameter, and resulted in systematic changes in magnetic susceptibility and specific heat. Stoichiometric and high quality single crystals of $rm Pr_2Zr_2O_7$ were grown using the optical floating zone technique under a high purity static argon atmosphere, to avoid inclusions of Pr$^{4+}$ and limit Pr vaporization. Increasing the growth speed was found to significantly reduce Pr vaporization for better control of stoichiometry. Scanning electron microscopy provided direct evidence of spinodal decomposition during growth that is controllable via rotation rate. An intermediate rotation rate of 3-6 rpm was found to produce the best microstructure. The magnetic susceptibility of crystals grown at rates from 1-20 mm/hr revealed changes that were consistent with Pr vaporization. Further, we report indications of local off-centering of Pr$^{3+}$ ions from the ideal pyrochlore sites, similar to what is known for the trivalent cation in $rm Bi_2Ti_2O_7$ and $rm La_2Zr_2O_7$. The effect varies with Pr content and radically modulates the low temperature specific heat. Overall, the results clearly demonstrate important correlations between the growth conditions and physical properties of $rm Pr_2Zr_2O_7$ crystals.
A novel macroscopically degenerate state called kagome ice, which was recently found in a spin ice compound Dy2Ti2O7 in a magnetic field applied along the [111] direction of the cubic unit cell, is studied by specific heat measurements. The residual entropy of the kagome ice is estimated to be 0.65 J/K mol Dy, which is nearly 40 % of that for the tetrahedral spin ice obtained in a zero field (1.68 J/K mol Dy) and is in good agreement with a theoretical prediction. It is also reported that the kagom ice state, which is stabilized at a range of magnetic field of 0.3 ~ 0.6 T, is a gas phase and condenses into a liquid phase with nearly zero entropy at a critical field of 1 T.
We use numerical linked cluster (NLC) expansions to compute the specific heat, C(T), and entropy, S(T), of a quantum spin ice model of Yb2Ti2O7 using anisotropic exchange interactions recently determined from inelastic neutron scattering measurements and find good agreement with experimental calorimetric data. In the perturbative weak quantum regime, this model has a ferrimagnetic ordered ground state, with two peaks in C(T): a Schottky anomaly signalling the paramagnetic to spin ice crossover followed at lower temperature by a sharp peak accompanying a first order phase transition to the ferrimagnetic state. We suggest that the two C(T) features observed in Yb2Ti2O7 are associated with the same physics. Spin excitations in this regime consist of weakly confined spinon-antispinon pairs. We suggest that conventional ground state with exotic quantum dynamics will prove a prevalent characteristic of many real quantum spin ice materials.
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