Investigating the order–disorder phase transition in Nd2−xYxZr2O7via diffraction and spectroscopy

Abstract

The pyrochlore–defect fluorite phase transition in the mixed-metal zirconate Nd_2−xY_xZr₂O₇ (0 ≤ x ≤ 2) solid solution was investigated using synchrotron X-ray and neutron diffraction, as well as X-ray absorption spectroscopy. Diffraction analysis revealed a two-phase region between 1.0 ≤ x ≤ 1.2. In the pyrochlore phase, Zr L₃-edge XANES analysis demonstrated a gradual change in the local coordination environment of the B site with increasing Y content that was consistent with an increase in disorder. Although Y L₃-edge XANES analysis suggested that the Y cations remained in an ordered coordination environment in the pyrochlore phase, disorder did gradually increase once the fluorite phase formed. It was found that Y cations prefer an ordered coordination environment near the phase boundary whereas Zr cations prefer a disordered coordination environment.