The boson peak in silicate glasses: insight from molecular dynamics

• Published in: Physical chemistry chemical physics : PCCP Vol. 25; no. 45; pp. 3127 - 3128
• Main Authors: El Hamdaoui, Ahmed, Ghardi, El Mehdi, Atila, Achraf, Jabraoui, Hicham, Badawi, Michael, Hasnaoui, Abdellatif, Ouaskit, Said
• Format: Journal Article
• Language: English
• Published: Cambridge Royal Society of Chemistry 22.11.2023
• Subjects: Alkali metals; Density of states; Elastic properties; Lithium oxides; Molecular dynamics; Vibration mode
• ISSN: 1463-9076; 1463-9084; 1463-9084
• DOI: 10.1039/d3cp02912c

In the low-frequency regime, 1 THz, glasses show an anomalous excess in their vibrational density of states called the boson peak (BP). The origin of BP has been a subject of debate since its first discovery a few decades ago. Although BP has been the focus of numerous studies, no conclusive answers have been found about its origins, which remained elusive to date. Here, we present results based on molecular dynamics of several binary and ternary silicate glasses with different network intermediates and modifier oxides. The vibrational density of states and the BP are reported for all the studied glasses. Their correlation with the elastic constant C 44 , structural, and dynamical properties are extensively discussed in terms of Voronoi atomic volume and the vibrational mean square displacement of Q 4 species specifically. We also question the classical classification of alkali oxides as modifiers, and we suggest that Li 2 O plays the role of pseudo-intermediate oxide in lithium silicate glasses. This claim is supported by the effect of Li on various vibrational modes, and this effect differs from the other alkali metals. Furthermore, we demonstrate a correlation between the BP intensities and both the Voronoi volume of the Q 4 and Q 3 units and vibrational mean square displacements. The correlation between the boson peak intensities, the structural and elastic properties of silicate glasses (ternary and binary systems) are discussed in addition to an anomalous behavior of lithium compared to the other alkali oxide modifiers.