Double interplay between localized vs. itinerant, ferro- vs. antiferromagnetism in Ge doped FeGa3

A comprehensive investigation on the complex magnetic properties of the FeGa3-xGex system is presented through a combination of Density Functional Theory, 57Fe Mossbauer spectroscopy and magnetic susceptibility. Spin density diagrams evidence the emergence of localized magnetic moments on the Fe atoms that leads to a majority ferromagnetic response in the samples with increasing Ge concentration, however, the distribution of magnetic moments is strongly dependent on the dopant configurations (which break the single Fe site symmetry) and in certain cases Fe moments aligned antiparallel are found. We discuss the combined theoretical and experimental results in terms of a scenario wherein increasing Ge-doping leads to an evolution from mostly localized moments at small concentrations to a combination of both localized and itinerant moments with different values in the magnetically ordered state (0.13 < x < 0.41), which can be described as ferromagnetic with a fragile antiferromagnetic component.