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Structure of liquid and glassy materials from ambient to extreme conditions: a multiprobe approach


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Chirawatkul, P., 2010. Structure of liquid and glassy materials from ambient to extreme conditions: a multiprobe approach. Thesis (Doctor of Philosophy (PhD)). University of Bath.

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    Abstract

    The structure of molten Au0.81Si0.19, Au0.72Ge0.28 and Ag0.74Ge0.26 alloys with a composition at or near to the eutectic was investigated by using neutron diffraction (ND). The results suggest that the Au-Au distance in the alloys is similar to that of liquid Au, there is a preference for Au-Si bonds and show that there are pre-peaks in the total structure factors for Au0.72Ge0.28 and Ag0.74Ge0.26 at 1.3(2) and 1.6(3) ˚, A−1 respectively. The asymptotic decay of the pair correlation functions was found to agree both with a theoretical prediction based on simple pair potentials and a fractal model for metallic glasses. The structure of glassy (R2O3)0.2(Al2O3)0.2(SiO2)0.6, where R denotes Dy, Ho or a 50:50 mixture of Dy and Ho, was investigated by using the method of isomorphic substitution in ND, x-ray diffraction (XRD) and extended x-ray absorption fine structure (EXAFS) spectroscopy. The network is made from SiO4 tetrahedral units with a distribution of AlO4, AlO5 and AlO6 units giving an average coordination number of 4.5(1). There is a distribution of RO5, RO6, RO7, RO8 and RO9 units with an average coordination number of 7.2(3) and an average R-O distance of 2.33(2) ˚ A. The EXAFS results confirmed that Dy and Ho are isomorphic and were used to refine an RMC model of the structure. R-Al and R-Si nearest neighbour shells with average distances of 3.15(3) and 3.6(1) ˚A were required to fit the EXAFS results. The structure of glassy and liquid ZnCl2 was studied by using ND and XRD. The material has a network structure made from ZnCl4 tetrahedra units which is retained in the liquid at temperatures near to the boiling point. An increase of temperature promotes edge sharing connectivity as inferred from a decrease of the Zn-Zn nearest neighbour distance and average Zn-Cl coordination number. An EXAFS study on crystalline ZnCl2 at room temperature shows that Zn remains 4fold coordinated at pressures less than 1 GPa, is 4+2-fold coordinated at 2-4 GPa, and is 6-fold coordinated above 4 GPa. For liquid ZnCl2, Zn is 4-fold coordinated by Cl at a pressure of about 1 GPa and could be 6-fold coordinated at 2-3 GPa.

    Details

    Item Type Thesis (Doctor of Philosophy (PhD))
    CreatorsChirawatkul, P.
    Uncontrolled Keywordsstructure, aluminosilicate, liquid, x-ray diffraction, rare-earth, extreme condition, alloy, glass, neutron diffraction, exafs
    DepartmentsFaculty of Science > Physics
    Publisher StatementUnivBath_PhD_2010_P_Chirawatkul.pdf: © The Author
    StatusUnpublished
    ID Code24893

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