Supplemental Information Tailoring magnetism of multifunctional MnxGa films with giant perpendicular anisotropy L. J. Zhu, D. Pan, S. H. Nie, J. Lu, J. H. Zhaoa) State Key Laboratory of Superlattices and Microstructures,Institute of Semiconductors, Chinese Academy of Sciences, P. O. Box 912, Beijing 100083, China a)Author to whom correspondence should be addressed; Electronic mail: jhzhao@red.semi.ac.cn dislocation MnGa GaAs Supplamental Fig1. Cross-sectional IFFT-TEM image of MnGa/GaAs interface. The straight line guides the position of the interface, ellipse guides the position where dislocation appears. As show in Fig 1(g) in the revised manuscript, these films exhibit much short c-axis than bulks with the same composition probably due to tensile strains from epitaxy on GaAs since GaAs has longer a-axis (0.3988 nm) than MnGa bulk (0.3875~0.3927, ref 23). c first drops, consistent with the trend in bulks (ref 14,23) and films on GaN (ref. 21); while it slowly comes back toward bulk value when x further increases. To make clear the composition-dependence of c here, let us first consider such two factors: as x increases, (a) bulk c decreases, which mainly contributes the decreasing trend of c to films; (b) bulk a slowly increases toward a-value of GaAs (ref 23), which contributes a decreasing trend of tensile strains (or tetragonal distortion) to films, further decreasing the departure from bulk valve c, so c should slowly come back toward bulk value as x increases toward 3.0. However, just based on the two mutual compensated trends, it can not give a derivation from the monotonically decreasing trend because the bulk a of MnxGa keeps smaller than that of GaAs though a increases all the way as x increases. So there must be some other reason that influences the strains,or tetragonal distortion, or a, such that has influence on c. Actually, measured values of both a and c in the films should be greatly affected by the level of dislocation formed during tensile strain relaxation. The similar phenomenon was observed and discussed in the growth of FePt on TiN buffers and was named “domain matching epitaxy”, please see Trichy et al, APL 92,102504(2008). In our MnGa films, we also observed a high level of dislocation or “domain matching epitaxy”–like growth as a result of much smaller a value of MnxGa without strain (bulk) than that of GaAs. Supplemental Fig. 1 shows cross-sectional inverse fast Fourier transform (IFFT) transmission electron microscopy (TEM) image of MnGa/GaAs interface, from which a very high level dislocation of lattice can be found. However, the composition dependence of tensile strain relaxation through the dislocation is rather a complicated process. The detailed studies are beyond the scope of this letter. For summary, the non-monotonic composition dependence of c should be attributed to a combination of (a) x-induced c decrease in absence of consideration of strains; (b) x-induced a increase, further results in decrease of minus departure of c from bulk values; (c) complicated x-dependence of a and c induced by complicated x-dependence of tensile strain relaxation. However, detailed studies to quantitatively make clear how much on earth the three factors respectively determine the x-dependence of c, are beyond the scope of this letter.