Experimental and theoretical study of anomalous temperature dependence of phonons in Y2Ti2O7 pyrochlore

Abstract

We present Raman spectroscopic as well as first-principles theoretical studies of the temperature dependence of phonon spectra in the pyrochlore ${\mathrm{Y}}_{2}{\mathrm{Ti}}_{2}{\mathrm{O}}_{7}$. Our experimental results show that the frequencies of several phonons display anomalous softening upon cooling. Our theoretical calculations of the temperature dependence, via phonon self-energy corrections arising from cubic anharmonic interactions, lead to such anomalies but only for a couple of high-frequency phonon modes. Our work strongly supports the suggestion that anharmonic phonon-phonon interactions are strong in the pyrochlore titanates and that they are responsible for the phonon anomalies observed. The strong anharmonic effects are likely due to the presence of the vacant Wyckoff sites and the shifts of the oxygen atoms from their actual positions in the pyrochlore lattice. However, the theoretical calculations fail to explain the anomalous behavior of low and intermediate frequency modes observed in our experiments. It seems likely that a much more sophisticated, perhaps nonperturbative, treatment of the anharmonic interactions will be required for a full explanation of the anomalies.