A structural, spectroscopic, and computational investigation of Stryker's reagent, [HCu{P(C6H5)(3)}](6), and its isotopomers has provided new insights into the complex. Neutron diffraction shows that the hydrides are best described as edge bridging rather than face bridging. The combination of infrared and inelastic neutron scattering spectroscopies has allowed the location of most of the modes associated with the hydrides and their assignments. The structural and spectroscopic conclusions are supported by the ab initio studies of the complex.