Mg_y Ni (2 ≤ y ≤ 10) thin films covered with a Pd cap layer are hydrogenated in 1 0⁵ Pa H₂ between room temperature and 80 ° C and their dielectric function over(ε, ̃) is determined from reflection and transmission measurements. The hydrogenated Mg_y NiH_x thin films show a continuous shift of the optical absorption towards higher photon energies with increasing y. Comparison of the obtained dielectric functions with predictions from an effective medium theory show that a considerable doping of the Mg₂ NiH₄ host takes place at least for y ≤ 3.5 while no signature of MgH₂ is observed in that composition range in the optical spectra. This is in contrast to the predictions from the bulk phase diagram where a mixture of semiconducting Mg₂ NiH₄ (energy gap E_g = 1.6 eV) and MgH₂ (E_g = 5.6 eV) is expected.

The structural, optical and dc electrical properties of Mg _xAl_1-x (0.2 ≤ x ≤ 0.9) gradient thin films covered with Pd/Mg are investigated before and after exposure to hydrogen. We use hydrogenography, a novel high-throughput optical technique, to map simultaneously all the hydride forming compositions and the kinetics thereof in the gradient thin film. Metallic Mg in the Mg_xAl_1-x layer undergoes a metal-to-semiconductor transition and MgH₂ is formed for all Mg fractions x investigated. The presence of an amorphous Mg-Al phase in the thin film phase diagram enhances strongly the kinetics of hydrogenation. In the Al-rich part of the film, a complex H-induced segregation of MgH₂ and Al occurs. This uncommon large-scale segregation is evidenced by metal and hydrogen profiling using Rutherford backscattering spectrometry and resonant nuclear analysis based on the reaction ¹H(¹⁵N, αγ)¹²C. Besides MgH₂, an additional semiconducting phase is found by electrical conductivity measurements around an atomic [Al]/[Mg] ratio of 2 (x = 0.33). This suggests that the film is partially transformed into Mg(AlH₄)₂ at around this composition.