Rattler model of the boson peak at silica surfaces

Abstract

Recent experiments unveiled two new aspects of the low-energy excitation spectrum of silica glass-commonly termed as the "boson peak" region. The first is that at low temperature the silica surface exhibits a different, softer boson peak than the bulk. The second is a giant thermal blueshift of the surface boson peak frequency causing it to cross and overcome the bulk peak with increasing temperature. Here we present a simple lattice model that reproduces this behavior in all its aspects. Each site consists of rigid tetrahedral units softly connected so as to be able to rotate anharmonically as "rattlers" in their cages. As shown by simulations, the model dynamics exhibits a boson-like peak, which has lower frequency at the surface where rattlers have a weaker restoring force. Upon heating however the larger angular freedom of surface units allows them to rattle more than in the bulk, leading to a steeper frequency increase similar to experiment. © 2012 American Institute of Physics.