Vibrational Properties of Polyanionic Hydrides SrAl2H2 and SrAlSiH: New Insights into Al−H Bonding Interactions

The vibrational properties of the recently discovered aluminum hydrides SrAl2H2 and SrAlSiH have been investigated by means of inelastic neutron scattering (INS) and first-principles calculations. Both compounds contain Al-H units being part of a two-dimensional polyanionic layer, [(AlH)(AlH)]2- and [Si(AlH)]2-, respectively. The INS spectrum of SrAlSiH is characterized by very weakly dispersed Al-H modes with well-resolved overtones, while SrAl2H2 yields a solid-state dispersed phonon spectrum. The frequency of the stretching mode of the Al-H unit in SrAlSiH is the hitherto lowest observed for a terminal Al-H bond. At the same time, SrAlSiH displays the highest decomposition temperature known for an aluminum hydride compound. It is proposed that the stability of solid-state aluminum hydrides correlates inversely with the strength of Al-H bonding.