Structural anisotropy in Sb thin films

Sb thin films have attracted wide interest due to their tunable band structure, topological phases, high electron mobility, and thermoelectric properties. We successfully grow epitaxial Sb thin films on a closely lattice-matched GaSb(001) surface by molecular beam epitaxy. We find a novel anisotropic directional dependence on their structural, morphological, and electronic properties. The origin of the anisotropic features is elucidated using first-principles density functional theory (DFT) calculations. The growth regime of crystalline and amorphous Sb thin films was determined by mapping the surface reconstruction phase diagram of the GaSb(001) surface under Sb₂ flux, with confirmation of structural characterizations. Crystalline Sb thin films show a rhombohedral crystal structure along the rhombohedral (211) surface orientation parallel to the cubic (001) surface orientation of the GaSb substrate. At this coherent interface, Sb atoms are aligned with the GaSb lattice along the [ 1 ̄ 10 ] crystallographic direction but are not aligned well along the [110] crystallographic direction, which results in anisotropic features in reflection of high-energy electron diffraction patterns, misfit dislocation formation, surface morphology, and transport properties. Our DFT calculations show that the preferential orientation of the rhombohedral Sb (211) plane may originate from the GaSb surface, where Sb atoms align with the Ga and Sb atoms on the reconstructed surface. The formation energy calculations confirm the stability of the experimentally observed structures. Our results provide optimal film growth conditions for further studies of novel properties of Bi_1−xSb_x thin films with similar lattice parameters and an identical crystal structure, as well as functional heterostructures of them with III-V semiconductor layers along the (001) surface orientation, supported by a theoretical understanding of the anisotropic film orientation.