  A new class of strongly infrared active structures is identified for phase
III of compressed molecular H2 by constant-pressure ab initio molecular
dynamics and density-functional perturbation calculations. These are planar
quadrupolar structures obtained as a distortion of low-pressure quadrupolar
phases, after they become unstable at about 150 GPa due to a zone-boundary soft
phonon. The nature of the II-III transition and the origin of the IR activity
are rationalized by means of simple electrostatics, as the onset of a
stabilizing dipole-quadrupole interaction.
