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We report the magnetic and electrical properties in Mn-doped and undoped (Zn,Sn)As2 epilayers, that were annealed at slightly higher temperatures than the growth temperature. (Zn,Sn)As2 :Mn were epitaxially grown on InP (001) substrates at 300°C, and showed room-temperature ferromagnetism. The hole concentration, saturation magnetization and Curie temperature were measured and evaluated as a function of annealing temperature. The Curie temperature had a tendency to slightly increase at annealing temperatures up to 340°C, and completely disappeared at 400°C. The ferromagnetism could be attributed to hole-mediated ferromagnetism resulting from Mn ion substitutions at both the II-group Zn and IV-group Sn sites, especially from the large solubility of Mn2+ substitution at Zn sites. The disappearance of ferromagnetism may be explained by several types of mechanisms : migration of mobile interstitial Mn atoms, diffusion of substitutional Mn ions to the surface, substitution of interstitial Mn atoms on Zn vacancies, and formation of MnAs clusters. It is noteworthy that the growth of magnetic semiconductor thin films from substrate lattice matching is essential for avoiding magnetic secondary phases such as MnAs clusters.

Mn-doped ZnSnAs2 (ZnSnAs2 :Mn) thin films with 5.0 and 6.5% Mn composition were epitaxially grown by molecular beam epitaxy on InP (001) substrates. These films had a Curie temperature of 334 K, corresponding to room-temperature ferromagnetism. The local structures around Mn atoms in ZnSnAs2 :Mn were studied by analysis of the X-ray absorption fine-structure spectra. It was found that the Mn atoms substitute into Zn or Sn cation sites, and the Mn‒As bond length is 2.50 A, which is slightly smaller than the value of 2.53 A in a sphalerite (zinc-blende) ZnSnAs2 bulk crystal. The Mn‒As bond length in ZnSnAs2 :Mn is consistent with the value obtained from GaMnAs, and has a smaller value than that obtained from the zinc-blend MnAs thin films grown on a InP substrate.