Phonon anomalies and structural transition in spin ice Dy2Ti2O7: a simultaneous pressure-dependent and temperature-dependent Raman study

Abstract

We revisit the assignment of Raman phonons of rare-earth titanates by performing Raman measurements on single crystals of O18 isotope-rich spin ice inline image and nonmagnetic inline image pyrochlores and compare the results with their O16 counterparts. We show that the low-wavenumber Raman modes below 250 cm−1 are not due to oxygen vibrations. A mode near 200 cm−1, commonly assigned as F2g phonon, which shows highly anomalous temperature dependence, is now assigned to a disorder-induced Raman active mode involving Ti4+ vibrations. Moreover, we address here the origin of the ‘new’ Raman mode, observed below TC ~ 110 K in Dy2Ti2O7, through a simultaneous pressure-dependent and temperature-dependent Raman study. Our study confirms the ‘new’ mode to be a phonon mode. We find that dTC/dP = + 5.9 K/GPa. Temperature dependence of other phonons has also been studied at various pressures up to ~8 GPa. We find that pressure suppresses the anomalous temperature dependence. The role of the inherent vacant sites present in the pyrochlore structure in the anomalous temperature dependence is also discussed. Copyright © 2012 John Wiley & Sons, Ltd.