Low-temperature nucleation anomaly in silicate glasses shown to be artifact in a 5BaO·8SiO2 glass

Abstract

For over 40 years, measurements of the nucleation rates in a large number of silicate glasses have indicated a breakdown in the Classical Nucleation Theory at temperatures below that of the peak nucleation rate. The data show that instead of steadily decreasing with decreasing temperature, the work of critical cluster formation enters a plateau and even starts to increase. Many explanations have been offered to explain this anomaly, but none have provided a satisfactory answer. We present an experimental approach to demonstrate explicitly for the example of a 5BaO ∙ 8SiO₂ glass that the anomaly is not a real phenomenon, but instead an artifact arising from an insufficient heating time at low temperatures. Heating times much longer than previously used at a temperature 50 K below the peak nucleation rate temperature give results that are consistent with the predictions of the Classical Nucleation Theory. These results raise the question of whether the claimed anomaly is also an artifact in other glasses.

The breakdown of classical nucleation theory at low temperatures for silicate glasses has been a puzzle for decades. Here, Xia et al. show with a long-term experiment for the specific case of a barium-silicate glass that this anomaly is in fact an artifact arising from insufficient heating time.