Structural and optical properties of Mg2NiHx switchable mirrors upon hydrogen loading

• The structural, thermodynamic and optical properties of Mg2Ni thin films covered with Pd are investigatedupon exposure to hydrogen. Similar to bulk, thin films of metallic Mg2Ni take up 4 hydrogen per formula unitand semiconducting transparent Mg2NiH4−d is formed. The dielectric function e˜ of Mg2Ni and fully loadedMg2NiH4−d is determined from reflection and transmission measurements using a Drude-Lorentz parametrization.Besides the two “normal” optical states of a switchable mirror—metallic reflecting and semiconductingtransparent—Mg2NiHx exhibit a third “black” state at intermediate hydrogen concentrations with low reflectionand essentially zero transmission. This state originates from a subtle interplay of the optical properties of theconstituent materials and a self-organized double layering of the film during loading. Mg2NiH4−d preferentiallynucleates at the film/substrate interface and not—as intuitively expected—close to the catalytic Pd cappinglayer. Using e˜Mg2Ni and e˜Mg2NiH4and this loading sequence, the optical response at all hydrogen concentrationscan be described quantitatively. The uncommon hydrogen loading sequence is confirmed by x-ray diffractionand hydrogen profiling using the resonant nuclear reaction 1Hs15N,agd12C. Pressure-composition isothermssuggest that

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