Structural properties of Y2O3–Al2O3 liquids and glasses: An overview

Abstract

Liquids in the system Y2O3−Al2O3 have been the subject of considerable study because of the reported occurrence of a first-order density and entropy-driven liquid–liquid phase transition (LLPT) in the supercooled liquid state. The observations have become controversial because of the presence of crystalline material that can be formed simultaneously and that can mask the nucleation and growth of the lower density liquid. The previous work is summarized here along with arguments for and against the different viewpoints. Also two studies have been undertaken to investigate the LLPT in this refractory system with emphasis on determining the structure of unequivocally amorphous materials. These include the in situ high energy X-ray diffraction (HEXRD) of supercooled Y2O3−Al2O3 liquids and the low frequency vibrational dynamics of recovered glasses. Many-body molecular dynamics simulations are also used to interpret the results of both studies. The HEXRD measurements, combined with aerodynamic levitation and rapid data acquisition techniques, show that for the 20mol% Y2O3 (i.e. AlY20) liquid there is a shift in the position of the first peak in the diffraction pattern over a narrow temperature range (2100–1800K) prior to crystallization. Microbeam Raman spectroscopy measurements made on AlY20 glasses clearly show contrasting spectra in the low frequency part of the spectrum for low- (LDA) and high-density (HDA) glassy regions. The molecular dynamics simulations identify contrasting coordination environments around oxygen anions for the high- (HDL) and low-density (LDL) liquids.