The vibrational dynamics of vitreous silica: Classical force fields vs. first principles
Laboratoire des Verres, Université Montpellier II -
34090 Montpellier, France
Accepted: 25 July 2002
We compare the vibrational properties of model SiO2 glasses generated by molecular-dynamics simulations using the effective force field of van Beest et al. (BKS) with those obtained when the BKS structure is relaxed using an ab initio calculation in the framework of the density functional theory. We find that this relaxation significantly improves the agreement of the density of states with the experimental result. For frequencies between 14 and 26 THz, the nature of the vibrational modes as determined from the BKS model is very different from the one from the ab initio calculation, showing that the interpretation of the vibrational spectra in terms of calculations using effective potentials can be very misleading.
PACS: 71.15.Pd – Molecular dynamics calculations (Car-Parrinello) and other numerical simulations / 61.43.Fs – Glasses / 61.20.Ja – Computer simulation of liquid structure
© EDP Sciences, 2002