Competing Ferromagnetic and Anti-Ferromagnetic interactions in Iron Nitride $\zeta$-Fe$_2$N

Abstract

The paper discusses the magnetic state of zeta phase of iron nitride viz. $\zeta$-Fe$_2$N on the basis of spin polarized first principles electronic structure calculations together with a review of already published data. Results of our first principles study suggest that the ground state of $\zeta$-Fe$_2$N is ferromagnetic (FM) with a magnetic moment of 1.528 $\mu_\text{B}$ on the Fe site. The FM ground state is lower than the anti-ferromagnetic (AFM) state by 8.44 meV and non-magnetic(NM) state by 191 meV per formula unit. These results are important in view of reports which claim that $\zeta$-Fe$_2$N undergoes an AFM transition below 10K and others which do not observe any magnetic transition up to 4.2K. We argue that the experimental results of AFM transition below 10K are inconclusive and we propose the presence of competing FM and AFM superexchange interactions between Fe sites mediated by nitrogen atoms, which are consistent with Goodenough-Kanamori-Anderson rules. We find that the anti-ferromagnetically coupled Fe sites are outnumbered by ferromagnetically coupled Fe sites leading to a stable FM ground state. A Stoner analysis of the results also supports our claim of a FM ground state.