Crystal-like low frequency phonons in the low-density amorphous and high-density amorphous ices

Abstract

The structure and vibrational properties of high- and low-density amorphous (HDA and LDA, respectively) ices have been determined using reverse Monte Carlo, molecular dynamics, and lattice dynamics simulations. This combined approach leads to a more accurate and detailed structural description of HDA and LDA ices when compared to experiment than was previously possible. The water molecules in these ices form well connected hydrogen-bond networks that exhibit modes of vibration that extend throughout the solid and can involve up to 70% of all molecules. However, the networks display significant differences in their dynamical behavior. In HDA, the extended low-frequency vibrational modes occur in dense parallel two dimensional layers of water that are approximately 10 nm thick. In contrast, the extended modes in LDA resemble a holey structure that encapsulates many small pockets of nonparticipating water molecules.