Goldstone-mode phonon dynamics in the pyrochlore Cd2Re2O7

We have measured the polarized Raman scattering spectra of Cd2Re2O7, the first superconducting pyrochlore, as a function of temperature. For temperatures below the cubic-to-tetragonal structural phase transition (SPT) at 200 K, a peak with B1 symmetry develops at zero frequency with divergent intensity. We identify this peak as the first observation of the Goldstone phonon in a crystalline solid. The Goldstone phonon is a collective excitation that exists due to the breaking of the continuous symmetry with the SPT. Its emergence coincides with that of a Raman-active soft mode. The order parameter for both features derives from an unstable doubly degenerate vibration (with Eu symmetry) of the O1 atoms which drives the SPT.