Local ordering and magnetism in Ga0.9Fe3.1N

Prior investigations of the ternary nitride series Ga1-xFe3+xN (0 <= x 1) have indicated a transition from ferromagnetic gamma'-Fe4N to antiferromagnetic ``GaFe3N''. The ternary nitride ``GaFe3N'' has been magnetically and spectroscopically reinvestigated in order to explore the weakening of the ferromagnetic interactions through the gradual incorporation of gallium into gamma'-Fe4N. A hysteretic loop at RI reveals the presence of a minority phase of only 0.1-0.2 at\%, in accord with the sound two-step synthesis. The composition of the gallium-richest phase ``GaFe3N'' was clarified by Prompt Gamma-ray Activation Analysis and leads to the berthollide formula Ga0.91(1)Fe3.09(10)N1.05(7). Magnetic measurements indicate a transition around 8 K, further supported by Mossbauer spectral data. The weakening of the ferromagnetic coupling through an increasing gallium concentration is explained by a simple Stoner argument. In Ga0.9Fe3.1N the presence of iron on the gallium site affects the magnetism by the formation of 13-atom iron clusters. (C) 2011 Elsevier Inc. All rights reserved.