Department of Materials Science and Engineering, Rensselaer Polytechnic Institute, Troy, New York 12180, USA.
Geophysical Laboratory, Carnegie Institution of Washington, Washington, DC 20015, USA.
J Chem Phys. 2018 May 21;148(19):194501. doi: 10.1063/1.5025592.
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.
拉曼和布里渊光散射技术被用于研究在热压缩(在 1100°C 时高达 8 GPa)下致密化的二氧化硅玻璃中热诱导的高密度非晶态(HDA)到低密度非晶态(LDA)的转变。结果表明,热压缩的二氧化硅样品在 600°C 或更高温度下保持结构和机械稳定性,与原始的二氧化硅玻璃相比,弹性响应对温度的敏感性降低。如果有足够的热能克服能垒,HDA 二氧化硅的致密结构将恢复到 LDA 状态。HDA 到 LDA 转变的起始温度取决于热压缩过程中的致密化程度,对于密度较高的样品,起始温度较低,但所有样品都在 250-300°C 的温度范围内完成。我们的研究表明,高温下热压缩样品中的 HDA 到 LDA 转变与冷压缩二氧化硅玻璃从室温开始的逐渐变化不同,这表明热压缩实现了更高的结构均匀性。此外,与非晶冰中突然的一级类似的多晶转变不同,热诱导的 HDA 到 LDA 转变过程中,热压缩二氧化硅玻璃的结构和性能不断变化。非晶态二氧化硅和非晶态冰中的不同 HDA 到 LDA 转变机制可以用它们不同的能量景观来解释。