Density-driven structural transformations in network forming glasses: a high-pressure neutron diffraction study of GeO2glass up to 17.5 GPa

Philip S Salmon, James W E Drewitt, Dean A J Whittaker, Anita Zeidler, Kamil Wezka, Craig L Bull, Matthew G Tucker, Martin C Wilding, Malcolm Guthrie, Dario Marrocchelli
2012 Journal of Physics: Condensed Matter  
2012) Density-driven structural transformations in network forming glasses: A high-pressure neutron diffraction study of GeO2 glass up to 17.5 GPa. Journal of Physics-Condensed Matter, 24 (41). ISSN 0953-8984 Link to official URL (if available): http://dx. Abstract. The structure of GeO 2 glass was investigated at pressures up to 17.5(5) GPa using in situ time-of-flight neutron diffraction with a Paris-Edinburgh press employing sintered diamond anvils. A new methodology and data correction
more » ... dure were developed, enabling a reliable measurement of structure factors that are largely free from diamond Bragg peaks. Calibration curves, which are important for neutron diffraction work on disordered materials, were constructed for pressure as a function of applied load for both single and double toroid anvil geometries. The diffraction data are compared to new molecular-dynamics simulations made using transferrable interaction potentials that include dipole-polarization effects. The results, when taken together with those from other experimental methods, are consistent with four densification mechanisms. The first, at pressures up to ≃5 GPa, is associated with a reorganization of GeO 4 units. The second, extending over the range from ≃5 to 10 GPa, corresponds to a regime where GeO 4 units are replaced predominantly by GeO 5 units. In the third, as the pressure increases beyond ∼10 GPa, appreciable concentrations of GeO 6 units begin to form and there is a decrease in the rate of change of the intermediate-range order as measured by the pressure dependence of the position of the first sharp diffraction peak. In the fourth, at about 30 GPa, the transformation to a predominantly octahedral glass is achieved and further densification proceeds via compression of the Ge-O bonds. The observed changes in the measured diffraction patterns for GeO 2 occur at similar dimensionless number densities to those found for SiO 2 , indicating similar densification mechanisms for both glasses. This implies a
doi:10.1088/0953-8984/24/41/415102 pmid:22951604 fatcat:d2loryzd2beinlcimgxvzx6ez4