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.

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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.

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The optical properties of Mg-TM (TM: Ni, Co, Fe; Mg:TM ≈ 2) thin films during hydrogenation are investigated using reflection and transmission measurements. Mg-Ni and Mg-Co show an unusual behavior upon exposure to hydrogen. The nucleation of the hydride starts at the film substrate interface and not - as intuitively expected - at the Pd covered top side of the film. Consequently, a double layer structure is formed. Reflection measurements are used to identify the loading behavior as the double layering yields to an remarkable optical black state at intermediate hydrogen concentrations. Photometric measurements on samples loaded at H2-pressures of 10 5 Pa show that in Mg-NiHx and Mg-CoHx the complex hydrides Mg2NiH4 and Mg2CoH5 are formed, whereas in Mg-Fex the formation of MgH2 is prevalent.@en