Thermodynamic modeling of fluid polyamorphism in hydrogen at extreme conditions

Abstract

Fluid polyamorphism, the existence of multiple amorphous fluid states in a single-component system, has been observed or predicted in a variety of substances. A remarkable example of this phenomenon is the fluid–fluid phase transition (FFPT) in high-pressure hydrogen between insulating and conducting high-density fluids. This transition is induced by the reversible dimerization/dissociation of the molecular and atomistic states of hydrogen. In this work, we present the first attempt to thermodynamically model the FFPT in hydrogen at extreme conditions. Our predictions for the phase coexistence and the reaction equilibrium of the two alternative forms of fluid hydrogen are based on experimental data and supported by the results of simulations. Remarkably, we find that the law of corresponding states can be utilized to construct a unified equation of state combining the available computational results for different models of hydrogen and the experimental data.