Solid molecular hydrogen: The Broken Symmetry Phase

By performing constant-pressure variable-cell ab initio molecular dynamics simulations we find a quadrupolar orthorhombic structure, of \(Pca2_1\) symmetry, for the broken symmetry phase (phase II) of solid H2 at T=0 and P =110 - 150 GPa. We present results for the equation of state, lattice parameters and vibronic frequencies, in very good agreement with experimental observations. Anharmonic quantum corrections to the vibrational frequencies are estimated using available data on H2 and D2. We assign the observed modes to specific symmetry representations.