Our report of a novel cationic dipalladium(I) hydride in (Angew. Chem. Int. Ed. 2010, 49, 6315) shows a linear Pd-Pd-H core with H-ligand dynamics (solution NMR). Ab-initio MD simulations for the isolated molecule show H transfer between Pd centres via a Pd-H-Pd core (timescale 2ps at 300K), and because differences between the measured molecular geometry in the crystal and our isolated-molecule calculation are slight, this transfer may also occur in the solid-state. This is difficult to confirm experimentally, but because substantial ligand dynamics involved, a comparison of the observed and calculated (crystal and gas-phase) INS will support, or refute, our MD showing H-transfer. Use of normal and ligand-deuterated samples will enable separation of H-ligand vibrational dynamics. This is important to understanding of a catalytic processes involving polynuclear Pd-H species.