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Considerable efforts have been devoted recently to synthesizing diluted magnetic semiconductors having ferromagnetic properties at room temperature because of their technological impacts for spintronic devices. In 2001 successful growth of GaMnN films showing room temperature ferromagnetism and p-type conductivity was reported. The estimated Curie temperature was 940 K at 5.7% of Mn, which is the highest among diluted magnetic semiconductors ever reported. However, the electronic mechanism behind the ferromagnetic behaviour has still been controversial. Here we show experimental evidence using ferromagnetic samples that Mn atoms are substitutionally dissolved into the GaN lattice and they exhibit mixed valences of +2 (majority) and +3. The p-type carrier density decreases significantly at very low temperatures. At the same time, magnetization dramatically decreases. The results imply that the ferromagnetic coupling between Mn atoms is mediated by holes in the mid-gap Mn band.

Room temperature ferromagnetism of GaMnN thin films is awaked by a mild hydrogenation treatment of samples synthesized by molecular beam epitaxy. Local environment of Mn atoms is monitored by Mn-L2,3 near edge x-ray absorption fine structure (NEXAFS) technique. Doped Mn ions are present at substitutional sites of Ga both before and after the hydrogenation. No secondary phase can be detected. Major valency of Mn changes from +3 to +2 by the hydrogenation. The present result supports the model that the ferromagnetism occurs when Mn2+ and Mn3+ are coexistent and holes in the mid- gap Mn band mediate the magnetic coupling.Comment: 12 pages, 5 figure

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