Path Integral Molecular Dynamics Simulation on Atomic Distribution in Amorphized Ice Ic

Abstract

We have investigated the effects of compression and quantization on atomic distribution in ice Ic and in its compressed states at 77 K and 10 K, using the path integral molecular dynamics (PIMD) simulations over wide range of volume. It has been found that the high density amorphous ice (HDA) is attained by compression but volume range to retain ice structure is wider at 10 K than 77 K. We have discovered that quantum dispersion of atoms in ice Ic at 10 K induces non-zero probability that hydrogen-bonded H 2 O molecular molecules are oriented nonlinearly in the crystal structure, which was believed to contain exclusively linear orientation of hydrogen-bonded molecular pairs in this ice. It has been found that for HDA there is each non-zero probability of orientational disorder of hydrogen-bonded H 2 O pairs, of such uniform distribution of H atoms as observed in supercritical fluids in general, and of H atoms located at the O-O midpoint. The present PIMD simulations have revealed that these observed anomalous characteristics of atomic distribution in HDA are caused by both quantization of atoms and compression of the system.