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High-pressure Raman study on the superconducting pyrochlore oxide Cd2Re2O7

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 Publication date 2018
  fields Physics
and research's language is English




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The superconducting pyrochlore oxide Cd2Re2O7 (Tc = 1 K), which is now considered as a candidate of the spin-orbit-coupled metal, shows an inversion-symmetry-breaking structural transition at Ts1 = 200 K. Ts1 decreases with increasing pressure and disappears at around Pc = 4:2GPa, where at least four high-pressure phases with tiny structural distortions are suggested by means of powder X-ray diffraction [Yamaura PRB 2017]. We have carried out Raman scattering experiments to investigate changes in the crystal symmetry under high pressures up to 4.8 GPa. A structural transition at 1.9-3.0 GPa and the recovery of inversion symmetry above Pc are observed at 12 K.



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Superconducting and structural phase transitions in a pyrochlore oxide Cd2Re2O7 are studied under high pressure by x-ray diffraction and electrical resistivity measurements. A rich P-T phase diagram is obtained, which contains at least two phases with the ideal and slightly distorted pyrochlore structures. It is found that the transition between them is suppressed with increasing pressure and finally disappears at a critical pressure Pc = 3.5 GPa. Remarkable enhancements in the residual resistivity as well as the coefficient A of the AT 2 term in the resistivity are found around the critical pressure. Superconductivity is detected only for the phase with the structural distortion. It is suggested that the charge fluctuations of Re ions play a crucial role in determining the electronic properties of Cd2Re2O7.
The superconducting pyrochlore oxide Cd2Re2O7 is revisited with a particular emphasis on the sample-quality issue. The compound has drawn attention as the only superconductor (Tc = 1.0 K) that has been found in the family of {alpha}-pyrochlore oxides since its discovery in 2001. Moreover, it exhibits two characteristic structural transitions from the cubic pyrochlore structure, with the inversion symmetry broken at the first one at 200 K. Recently, it has attracted increasing attention as a candidate spin-orbit coupled metal (SOCM), in which specific Fermi liquid instability is expected to lead to an odd-parity order with spontaneous inversion-symmetry breaking [L. Fu, Phys. Rev. Lett. 115, 026401 (2015)] and parity-mixing superconductivity [V. Kozii and L. Fu: Phys. Rev. Lett. 115 (2015) 207002; Y. Wang et al., Phys. Rev. B 93 (2016) 134512]. We review our previous experimental results in comparison with those of other groups in the light of the theoretical prediction of the SOCM, which we consider meaningful and helpful for future progress in understanding this unique compound.
Rattling-induced superconductivity in the {beta}-pyrochlore oxide KOs2O6 is investigated under high pressure up to 5 GPa. Resistivity measurements in a high-quality single crystal reveal a gradual decrease in the superconducting transition temperature Tc from 9.7 K at 1.0 GPa to 6.5 K at 3.5 GPa, followed by a sudden drop to 3.3 K at 3.6 GPa. Powder X-ray diffraction experiments show a structural transition from cubic to monoclinic or triclinic at a similar pressure. The sudden drop in Tc is ascribed to this structural tran-sition, by which an enhancement in Tc due to a strong electron-rattler interaction present in the low-pressure cubic phase is abrogated as the rattling of the K ion is completely suppressed or weakened in the high-pressure phase of reduced symmetry. In addition, we find two anomalies in the temperature dependence of resistivity in the low-pressure phase, which may be due to subtle changes in rattling vibration.
The successive phase transitions of the pyrochlore oxide Cd2Re2O7 are studied by polarizing microscopy and magnetic susceptibility measurements. The formation of twin domains is visualized in the polarizing images of a pristine (111) crystal surface upon cooling through the cubic-to-tetragonal transition at Ts1 ~ 200 K. Moreover, a dramatic change in the twinning pattern is observed at Ts2 ~120 K, which suggests that the tetragonal c axis flips as the strain changes its direction at the tetragonal-to-tetragonal transition. Magnetic susceptibility measurements reveal significant domain alignment upon cooling across Ts1 and Ts2 in a magnetic field of 7 T, which are due to ~10% anisotropy in the magnetic susceptibility for the low-temperature phases. Interestingly, the anisotropy is reversed at Ts2: c{hi}c < c{hi}a above Ts2 and vice versa below Ts2.
The 5d pyrochlore oxide Cd2Re2O7 exhibits successive phase transitions from a cubic pyrochlore structure (phase I) to a tetragonal structure without inversion symmetry below Ts1 of ~200 K (phase II) and further to another noncentrosymmetric tetragonal structure below Ts2 of ~120 K (phase III). The two low-temperature phases may be characterized by odd-parity multipolar orders induced by the Fermi liquid instability of the spin-orbit-coupled metal. To control the tetragonal domains generated by the transitions and to obtain a single-domain crystal for the measurements of anisotropic properties, we prepared single crystals with the (0 0 1) surface and applied biaxial and uniaxial stresses along the plane. Polarizing optical microscopy observations revealed that inducing a small strain of approximately 0.05% could flip the twin domains ferroelastically in a reversible fashion at low temperatures, which evidences that the tetragonal deformation switches at Ts2 between c > a for phase II and c < a for phase III. Resistivity measurements using single-domain crystals under uniaxial stress showed that the anisotropy was maximum at around Ts2 and turned over across Ts2: resistivity along the c axis is larger (smaller) than that along the a axis by ~25% for phase II (III) at around Ts2. These large anisotropies probably originate from spin-dependent scattering in the spin-split Fermi surfaces of the cluster electric toroidal quadrupolar phases of Cd2Re2O7.
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