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Controlling electronic population through chemical doping is one way to tipthe balance between competing phases in materials with strong electroniccorrelations. Vanadium dioxide exhibits a first-order phase transition ataround 338 K between a high temperature, tetragonal, metallic state (T) and alow temperature, monoclinic, insulating state (M1), driven by electron-electronand electron-lattice interactions. Intercalation of VO2 with atomic hydrogenhas been demonstrated, with evidence that this doping suppresses thetransition. However, the detailed effects of intercalated H on the crystal andelectronic structure of the resulting hydride have not been previouslyreported. Here we present synchrotron and neutron diffraction studies of thismaterial system, mapping out the structural phase diagram as a function oftemperature and hydrogen content. In addition to the original T and M1 phases,we find two orthorhombic phases, O1 and O2, which are stabilized at higherhydrogen content. We present density functional calculations that confirm themetallicity of these states and discuss the physical basis by which hydrogenstabilizes conducting phases, in the context of the metal-insulator transition.

In situ diffraction study of catalytic hydrogenation of VO2: Stable phases and origins of metallicity