Calculation of the raman frequency, damping constant (Linewidth) and the relaxation time near the tetragonal-cubic transition in PbTiO3

Abstract

Frequencies, damping constants and the relaxation times of some Raman modes including the two soft modes are calculated as a function of pressure near the tetragonal-cubic transition in PbTiO3. Calculation of the Raman frequencies is performed using the observed volume data from the literature by means of the mode Gruneisen parameter at various pressures. Pressure dependence of the damping constant and the relaxation time is predicted using the pseudospin-phonon coupled model and the energy fluctuation model by considering that the Raman frequency can be taken as the order parameter (spontaneous polarization) for the tetragonal-cubic transition in PbTiO3. Expressions from both models for the damping constants are fitted to the observed Raman linewidths of the two soft modes and for the other Raman modes the damping constant and the relaxation time are predicted close to the transition. We find that damping constants diverge and the inverse relaxation time decreases for the soft modes with increasing pressure near the critical pressure (P-c similar to 11 GPa). The other Raman modes exhibit unusual critical behavior. Our results indicate that the observed behavior of the Raman frequencies can be predicted from the volume data through the mode Gruneisen parameter for the tetragonal-cubic transition in PbTiO3. The damping constant and the relaxation time for the Raman modes can also be predicted adequately using the pseudospin-phonon coupled model and the energy fluctuation model to explain the mechanism of the phase transition between the tetragonal and cubic phases in PbTiO3. (C) 2017 Elsevier GmbH. All rights reserved.