Pressure dependence of the monoclinic phase in (1-x)Pb(Mg1/3Nb2/3)O3-xPbTiO3 solid solutions

TL;DR

This study investigates how pressure affects the monoclinic phase in PMN-xPT solid solutions using multiple high-pressure techniques, revealing phase transitions and domain behavior up to 20 GPa.

Contribution

It provides the first comprehensive pressure-dependent phase diagram for PMN-xPT solid solutions, highlighting the persistence of monoclinic symmetry under high pressure.

Findings

Monoclinic phase persists up to 7 GPa in the morphotropic region.

Structural phase transition occurs above 6 GPa, merging diffraction peaks.

Ferroelectric domains diminish and vanish at around 3 GPa.

Abstract

We combine high-pressure x-ray diffraction, high-pressure Raman scattering, and optical microscope to investigate a series of PMN-xPT solid solutions (x=0.2, 0.3, 0.33, 0.35, 0.37, 0.4) in diamond anvil cells up to 20 GPa at 300 K. The Raman spectra show a peak centered at 380 cm-1 above 6 GPa for all samples, in agreement with previous observations. X-ray diffraction measurements are consistent with this spectral change indicating structural phase transition; we find that the triplet at the pseudo cubic (220) Bragg peak merges into a doublet above 6 GPa. Our results indicate that the morphotropic phase boundary region (x=0.33 to 0.37) with the presence of monoclinic symmetry persists up to 7 GPa. The pressure dependence of ferroelectric domains in PMN-0.32PT single crystals was observed using a polarizing optical microscope. The domain wall density decreases with pressure and domains disappear at a modest pressure of 3 GPa. We propose a pressure-composition phase diagram for PMN-xPT solid solutions.