Michael Guerette

Structure and Properties of Silica Glass Densified in Cold Compression and Hot Compression.

Silica glass has been shown in numerous studies to possess significant capacity for permanent densification under pressure at different temperatures to form high density amorphous (HDA) silica. However, it is unknown to what extent the processes leading to irreversible densification of silica glass in cold-compression at room temperature and in hot-compression (e.g., near glass transition temperature) are common in nature. In this work, a hot-compression technique was used to quench silica glass from high temperature (1100 °C) and high pressure (up to 8 GPa) conditions, which leads to density increase of ~25% and Young’s modulus increase of ~71% relative to that of pristine silica glass at ambient conditions. Our experiments and molecular dynamics (MD) simulations provide solid evidences that the intermediate-range order of the hot-compressed HDA silica is distinct from that of the counterpart cold-compressed at room temperature. This explains the much higher thermal and mechanical stability of the former than the latter upon heating and compression as revealed in our in-situ Brillouin light scattering (BLS) experiments. Our studies demonstrate the limitation of the resulting density as a structural indicator of polyamorphism, and point out the importance of temperature during compression in order to fundamentally understand HDA silica.

A simple and convenient set-up for high-temperature Brillouin light scattering

An emulated platelet geometry (or reflection-induced platelet geometry) is employed to collect photons scattered from both longitudinal and transverse acoustic waves travelling within a bulk transparent sample sitting on a reflective Pt plate. Temperature of the sample was controlled with a Linkam TS1500 optical furnace (maximum temperature of 1500 °C). This simple and convenient set-up allows a full determination of elastic constants of transparent materials in situ as a function of temperature from Brillouin light scattering. Structural information can be gained at the same time by guiding the scattered light into a Raman spectrometer using a flipping mirror or a beam splitter. We will demonstrate the applications of this set-up in transparent inorganic glasses, but it can be easily extended to any other transparent materials, either crystalline or amorphous in nature.

Thermally induced amorphous to amorphous transition in hot-compressed silica glass

In situ Raman and Brillouin light scattering techniques were used to study thermally induced high-density amorphous (HDA) to low-density amorphous (LDA) transition in silica glass densified in hot compression (up to 8 GPa at 1100 °C). Hot-compressed silica samples are shown to retain structural and mechanical stability through 600 °C or greater, with reduced sensitivity in elastic response to temperature as compared with pristine silica glass. Given sufficient thermal energy to overcome the energy barrier, the compacted structure of the HDA silica reverts back to the LDA state. The onset temperature for the HDA to LDA transition depends on the degree of densification during hot compression, commencing at lower temperatures for samples with higher density, but all finishing within a temperature range of 250-300 °C. Our studies show that the HDA to LDA transition at high temperatures in hot-compressed samples is different from the gradual changes starting from room temperature in cold-compressed silica glass, indicating greater structural homogeneity achieved by hot compression. Furthermore, the structure and properties of hot-compressed silica glass change continuously during the thermally induced HDA to LDA transition, in contrast to the abrupt and first-order-like polyamorphic transitions in amorphous ice. Different HDA to LDA transition mechanisms in amorphous silica and amorphous ice are explained by their different energy landscapes.