A fresh look at dense hydrogen under pressure. I. An introduction to the problem, and an index probing equalization of H–H distances

Vanessa Labet (1) , Paulina Gonzalez-Morelos (1) , Roald Hoffmann (1) , N W Ashcroft (1)

1 Cornell University [New York]

In the first of a series of four papers on hydrogen under pressure, and its transitions from an initiating molecular state, we begin by defining carefully the problem, and setting the distance scale of interactions of protons and electrons in molecular aggregates of the first of the elements. Following a review of the experimental situation, in particular the phase diagram of hydrogen, in as much as it is known, and the behavior of its vibrons and rotons, we move onto the setting up of a numerical laboratory for probing the underlying physics and chemistry of interactions in hydrogen as the pressure increases. The laboratory consists of the preferred static structures emerging from calculations on the system in the range of 1 atm to 500 GPa, those of Pickard and Needs. The intermolecular (inter-pair) H · · · H separations naturally decrease with increasing pressure, first rapidly so, then more slowly. The intramolecular (intra-pair) H-H distances vary over a much smaller scale (0.05 Å) as the pressure increases, first decreasing, then increasing, and finally decreasing. We define an equalization function to gauge the approach to equality of the first neighbor and shortest next neighbor H (proton) separations in this numerical laboratory. And we find that metallization is likely to occur before bond equalization.

Domaines: Chimie théorique et/ou physique

Vanessa Labet, Paulina Gonzalez-Morelos, Roald Hoffmann, N W Ashcroft. A fresh look at dense hydrogen under pressure. I. An introduction to the problem, and an index probing equalization of H–H distances. Journal of Chemical Physics, 2012, 136, ⟨10.1063/1.3679662⟩. ⟨hal-02202225⟩