The electronic structure and magnetic properties of chalcopyrite (CH) AlGaAs2 with dopant Mn at 3.125 and 6.25 % concentrations are investigated using first-principles calculations. The CH AlGaAs2 alloy is a p-type semiconductor with a small band-gap. The AlGaAs2:Mn shows that the ferromagnetic (FM) state is the most energetically favorable one. The Mn-doped AlGaAs2 exhibits FM and strong half-metallic ground states.The spin polarized Al(Ga,Mn)As2 state (Al-rich system) is more stable than the (Al,Mn)GaAs2 state (Ga-rich system), which has a magnetic moment of 3.82mB/Mn. The interaction between Mn-3d and As-4p states at the Fermi level dominates the other states.The states at the Fermi level are mainlyAs-4p electrons, which mediate strong interaction between the Mn-3d and As-4p states. It is noticeable that the FM ordering of dopant Mn with high magnetic moment originates from the As(4p)-Mn(3d)-As(4p) hybridization, which is attributed to the partially unfilled As-4pbands. The high FM moment of Mn is due to the double-exchange mechanism mediated by valence-band holes.

Effects of oxygen deficiency on the room temperature ferromagnetism in Fe-doped reduced have been investigated by comparing the air-annealed compound with secondly post-annealed one in vacuum ambience. The air-annealed sample showed a paramagnetic behavior at room temperature. However, when the sample was further annealed in vacuum, a strongly enhanced ferromagnetic behavior was observed at same temperature. spectra of air-annealed sample at 295K showed a single doublet of , suggesting that the Fe ions are paramagnetic. On the other hand, the absorption spectra after vacuum-annealing exhibited two doublets, in which one is the same component with air-annealed sample and the other is new doublet corresponding to state. This result suggests that the occurrence of ferromagnetism in reduced sample may be interpreted as the contribution of unquenched orbital moment of ions.