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The 5d pyrochlore oxide superconductor Cd2Re2O7 (CRO) has attractedsignificant interest as a spin-orbit-coupled metal (SOCM) that spontaneouslyundergoes a phase transition to an odd-parity multipole phase by breaking thespatial inversion symmetry due to the Fermi liquid instability caused by strongspin-orbit coupling. Despite the significance of structural information duringthe transition, previous experimental results regarding lattice deformationhave been elusive. We have conducted ultra-high resolution synchrotronradiation x-ray diffraction experiments on a high-quality CRO single crystal.The temperature-dependent splitting of the 0 0 16 and 0 0 14 reflections, whichare allowed and forbidden, respectively, in the high-temperature cubic phase I(space group Fd-3m), has been clearly observed and reveals the followingsignificant facts: inversion symmetry breaking and tetragonal distortion occursimultaneously at Ts1 = 201.5(1) K; the previously believed first-ordertransition between phase II (I-4m2) and phase III (I4122) at Ts2 ~ 120 Kconsists of two close second-order transitions at Ts2 = 115.4(1) K and Ts3 ~100 K; there is a new orthorhombic phase XI (F222) in between. The orderparameters (OPs) of these continuous transitions are uniquely represented by atwo-dimensional irreducible representation Eu of the Oh point group, and theOPs of phase XI are a linear combination of those of phases II and III. Eachphase is believed to correspond to a distinct odd-parity multipole order, andthe complex successive transitions observed may be the result of an electronicphase transition that resolves the Fermi liquid instability in the SOCM.

Successive phase transitions of the spin-orbit-coupled metal Cd2Re2O7 probed by high-resolution synchrotron x-ray diffraction