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The properties of hydrogen at high pressure have wide implications inastrophysics and high-pressure physics. Its phase change in the liquid isvariously described as a metallization, H2-dissociation, density discontinuityor plasma phase transition. It has been tacitly assumed that these phenomenacoincide at a first-order liquid-liquid transition (LLT). In this work, therelevant pressure-temperature conditions are thoroughly explored withfirst-principles molecular dynamics. We show there is a large dependency onexchange-correlation functional and significant finite size effects. We usehysteresis in a number of measurable quantities to demonstrate a first-ordertransition up to a critical point, above which molecular and atomic liquids areindistinguishable. At higher temperature beyond the critical point,H2-dissociation becomes a smooth cross-over in the supercritical region thatcan be modelled by a pseudo-transition, where the H2-2H transformation islocalized and does not cause a density discontinuity at metallization.Thermodynamic anomalies and counter-intuitive transport behavior of protons arealso discovered even far beyond the critical point, making this dissociativetransition highly relevant to the interior dynamics of Jovian planets. Belowthe critical point, simulation also reveals a dynamic H2-2H chemicalequilibrium with rapid interconversion, showing that H2 and H are miscible. Thepredicted critical temperature lies well below the ionization temperature. Ourcalculations unequivocally demonstrate that there are three distinct regimes inthe liquid-liquid transition of warm dense hydrogen.

Thermodynamic anomalies and three distinct liquid-liquid transitions in warm dense liquid hydrogen