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 Pca2₁ symmetry for the broken symmetry phase (phase II) of solid H₂ at T0ex0ex=0ex0ex0 and P0ex0ex=0ex0ex110--150GPa. 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.