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Local structure around Gd in GdAl3Cl12 glass and supercooled liquid: a Gd LIII-edge EXAFS study

The coordination environment around Gd3+ ions in GdAl3 Cl12 glass and supercooled liquid has been studied using Gd LIII -edge EXAFS spectroscopy. The Gd coordination environment in the glass is found to be similar to that in the GdAl3 Cl12 crystal with eight Cl nearest neighbours and four Al next-nearest neighbours. The Gd-Cl distance in the glass is the same as that in the crystal (~2.8 Å) although the Gd-Al distance in the glass (~3.85 Å) is longer than that in the crystal (~3.7 Å), indicating a less dense structure with a larger Gd-Cl-Al bond angle in the former. The Gd-Cl distance and coordination number are found to remain unchanged in the supercooled liquid at 60 °C. However, the absence of any Gd-Al second-neighbour shell in the EXAFS spectrum of the liquid indicates substantial increase in static disorder in the spatial disposition of AlCl4 tetrahedra around Gd in the liquid. Such temperature dependent structural changes are suggested to be responsible for the marked fragility of this liquid.