Structural and dynamic properties of vitreous and crystalline barium disilicate: molecular dynamics simulation and Raman scattering experiments

Abstract

In this paper, we use a molecular dynamics simulation and Raman scattering measurements to study the vibrational and structural characteristics of barium disilicate, BaSi 2 O 5 , in vitreous and crystalline states. Our proposed atomic interaction potential describes the structural and dynamic behaviour of this material very well and can also be used for further extended studies. In addition, Raman spectroscopy enabled validation of the predictions of the potential by comparing the simulated vibrational density of states with the spectrum of the material in its vitreous state. Furthermore, we characterized the kinetics of the crystallization process through in situ Raman measurements as a function of temperature.

A Raman investigation of the structural evolution of supercooled liquid barium disilicate during crystallization

“…BS2 glass and supercooled liquid Raman spectra (SCL) have been previously reported in several studies . Our spectra are qualitatively the same as previous studies and are compared to L‐BS2 reference spectra (Figure ).…”

“…In contrast, the peaks at 920 and 1060 cm −1 remain at apparently constant positions while their intensities decrease and increase, respectively (Figures and ). The latter behavior is expected as the crystalline L‐BS2 has a single sharp peak near 1060 cm −1 (Figure ) …”

“…The sensitivity of Raman spectroscopy to monitor the BS2 crystallization process was shown by Rodrigues et al., however, the structural evolution of supercooled liquid and the crystallization process itself were not investigated. Raman spectroscopy is among the most sensitive techniques to the local and medium‐range order within silicate glasses and melts .…”

“…At low wave numbers, below ~250 cm −1 the Boson peak is observed in all amorphous silicate materials . Although its origin is still debated, it is a signature of the amorphous state whether as a glass or SCL . In silica‐poor alkaline earth‐bearing silicates, the region from 200 to 400 cm −1 is dominated by oxygen vibrations associated with the modifier polyhedra, whereas in silica‐rich compositions there are additional vibrations related to the bridging oxygen rocking and stretching vibrations .…”

“…[10][11][12] The role of these metastable phases in the crystal nucleation and growth processes is still poorly understood and warrants further investigation beyond this study. 2,7 The sensitivity of Raman spectroscopy to monitor the BS2 crystallization process was shown by Rodrigues et al, 13 however, the structural evolution of supercooled liquid and the crystallization process itself were not investigated. Raman spectroscopy is among the most sensitive techniques to the local and medium-range order within silicate glasses and melts.…”