Molecular beam epitaxy was used to deposit body centered cubic single crystal Fe1-xGax thin films on MgO(001) and ZnSe/GaAs(001) substrates well beyond the bulk stability concentration of about 28%. The crystal quality of the substrate surface and each deposited layer was monitored in situ by reflection high energy electron diffraction. The magnetization of the samples as a function of Ga is found to decrease more rapidly than a simple dilution effect, and element-specific x-ray magnetic circular dichroism ascribes this trend to a decrease in the Fe moment and an induced moment in the Ga that is antialigned to the Fe moment. (C) 2010 American Vacuum Society. [DOI: 10.1116/1.3447233]