Heavily carbon-doped Mn 5 Ge 3 is a unique compound for spintronics applications as it meets all the requirements for spin injection and detection in group-IV semiconductors. Despite the great improvement of the magnetic properties induced by C incorporation into Mn 5 Ge 3 compounds, very little information is available on its structural properties and the genuine role played by C atoms.In this paper, we have used a combination of advanced techniques to extensively characterize the structural and magnetic properties of Mn 5 Ge 3 C x films grown on Ge(111) by solid phase epitaxy as a function of C concentration. The increase of the Curie temperature induced by C doping up to 435 K is accompanied by a decrease of the out-of-plane c-lattice parameter. The Mn and C chemical environments and positions in the Mn 5 Ge 3 lattice have been thoroughly investigated usingx-ray absorption spectroscopy techniques (x-ray absorption near-edge structures and extended xray absorption fine structures) and scanning transmission electronic microscopy (STEM) combined to electron energy loss spectroscopy for the chemical analysis. The results have been systematically compared to a variety of structures that were identified as favorable in terms of formation energy by ab initio calculations. For x ≤ 0.5, the C atoms are mainly located in the octahedral voids formed by Mn atoms, which is confirmed by simulations and seen for the first time in real space by STEM. However, the latter reveals an inhomogeneous C incorporation, which is qualitatively correlated to the broad magnetic transition temperature. A higher C concentration leads to the formation of manganese carbide clusters that we identified as Mn 23 C 6 . Interestingly, other types of defects, such as interstitial Ge atoms, vacancies of Mn, and their association into line defects, have been detected. They take part in the strain relaxation process and are likely to be intimately related to the growth process. This paper provides a complete picture of the structure of Mn 5 Ge 3 C x in thin films grown by solid phase epitaxy, which is essential for optimizing their magnetic properties.
