Evidence of negative thermal expansion in supercooled tantala

Abstract

A density anomaly, i.e. a temperature region with negative thermal expansion (NTE) bounded by a density maximum and a density minimum at lower temperatures, is revealed and characterised in tantala for the first time by Molecular Dynamics simulations. The NTE region is evidenced in the metastable supercooled liquid and rather close to the glass transition. Since NTE is suppressed by poor structural equilibration, highlighting these phenomena is highly challenging due to the need for fulfilling competing constraints of slow cooling and avoidance of the crystallization. We find that the density anomaly is signalled by a decrease of the partial coordination numbers nTa,Ta and nO,O when lowering the temperature. The NTE magnitude is comparable to the ones of both stable water and solid-state materials with giant NTE.