Abstract
Correlation of crystal structure with electric field gradient (EFG) in the fluorite- and pyrochlore-type compounds in the Gd 2O 3–ZrO 2 system Gd x Zr 1− x O 2− x/2 with 0.18⩽ x⩽0.62 were investigated by 155Gd Mössbauer spectroscopy, powder X-ray diffraction and point-charge model (PCM) calculation. An intermediate ordered pyrochlore phase forms for 0.45⩽ x⩽0.55, sandwiched with a disordered fluorite phase for 0.18⩽ x<0.45 and 0.55< x⩽0.62. Some 155Gd Mössbauer parameters, especially the quadrupole coupling constant ( e 2 qQ), were found to exhibit a characteristic maximum around the ideal-pyrochlore Gd 2Zr 2O 7 ( x=0.50) composition. The validity of the proposed pyrochlore-based structural model was examined by comparing the experimental values of EFG at the Gd sites with those calculated by the PCM calculations.
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