Epitaxial single crystal thin films of U3Si, U3Si5, α−USi2, and USi3, alongside poly-crystalline U3Si2 have all been synthesised using DC magnetron sputtering. These idealised samples provide the bases on which fundamental studies can be conducted for understanding advanced technology fuel (ATF) candidates: U3Si2, U3Si5. The silicon-rich phases, USi2 USi3 are interest as intermediate oxidation ...