Epitaxial Growth of Anisotropic SnSe on GaAs(001) via Step-Edge Orientation Control

Epitaxial growth of orthorhombic SnSe on cubic substrates is challenging due to lattice-symmetry mismatch and anisotropic bonding. Here we demonstrate that epitaxial films with sharp interfaces can be achieved for layered SnSe grown directly on on-axis and 4 degree miscut GaAs(001) substrates. The substrate miscut strongly influences the growth morphology, evolving from spirals on on-axis GaAs to a terraced structure on miscut GaAs. X-ray diffraction reveals that on-axis GaAs supports SnSe with two in-plane orientation variants, whereas the miscut substrate stabilizes a single orientation and introduces a small out-of-plane tilt. Accordingly, in-plane optical anisotropy is enhanced in the single variant film compared to the double variant, as determined by cross-polar reflectance. High-resolution TEM shows that the SnSe/GaAs interface is atomically abrupt and incoherent, characteristic of quasi-van der Waals epitaxy. We find a pronounced tendency for the zigzag edges of SnSe to align parallel to step edges on both substrates, and we show that step-skipping nucleation and layer growth on the miscut substrate leads to the additional tilt. These results establish direct SnSe/GaAs heteroepitaxy as a route to integrate anisotropic layered semiconductors with cubic platforms, and show that miscut substrates provide additional control over in-plane anisotropy.