Negative thermal expansion in ice I polytypes

Abstract

The fundamental properties of ice have always attracted a lot of interest due to omnipresence of ice in many different natural contexts. Since cubic ice recently become experimentally accessible from a low-density gas hydrate precursor [1, 2], it has been possible to measure its density as a function of temperature in the whole thermodynamic range of metastability. We found strong analogies with respect to the other ice I polytype, i.e., hexagonal ice Ih [3], including the presence of a negative thermal expansion behavior at low temperature. Based on these results, a new enthalpy calculation quantifies the metastable nature of the cubic form and, consequently its inaccessibility from a "normal" ice Ih precursor.