Structure of Liquid Al6Si2O13 (3:2 Mullite) |
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Authors: | Shankar Krishnan J. Richard K. Weber Stuart Ansell April D. Hixson Paul C. Nordine |
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Affiliation: | Containerless Research, Inc., Evanston, Illinois 60201;and;European Synchrotron Radiation Facility (ESRF), Grenoble, France |
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Abstract: | We report the first measurements of the structure factor, S ( Q ), and the pair distribution function, G ( r ), of Al6Si2O13 (3:2 mullite) in the normal and supercooled liquid states in the temperature range 1776–2203 K. Measurements are obtained by synchrotron X-ray scattering on levitated, laser-heated liquid specimens. The S ( Q ) shows a prepeak at 2.0 Å−1 followed by a main peak at 4.5 Å−1 and a weak feature at 8 Å−1. The G ( r ) shows a strong (Si,Al)–O correlation at 1.80 Å at high temperature that moves to 1.72 Å as the liquid is supercooled. The second and third nearest neighbor peaks at 3.0 and 4.25 Å sharpen with supercooling. The short-range structure of the high-temperature liquid is similar to the corresponding glasses produced by rapid quenching. Supercooling causes an increase in the concentration of tetrahedral Si4+ ions, which is manifested by the large shift in the first peak to lower ionic distance, r , values in G ( r ). The increase in tetrahedrally coordinated Si4+ ions is offset by an increase in octahedral Al3+ ions. The clustering of the SiO44− tetrahedral units results in increased viscosity of the liquid at temperatures below the melting point, which is consistent with Al6Si2O13 being a fragile liquid. |
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