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Main-group chalcogenides with layered crystal structures and high in-planeanisotropy are attracting increasing interest for a range of practicalapplications. The III-VI semiconductor, monoclinic gallium monotelluride(m-GaTe), has been recently used in high-sensitivityphotodetectors/phototransistors and electronic memory applications due to itsanisotropic properties yielding superior optical and electrical performance.Despite these applications, the origin of such anisotropy, namely the complexstructural and bonding environments in GaTe nanostructures remain to be fullyunderstood. In the present work, we report a comprehensive atomic-scalecharacterization of m-GaTe by state-of-the-art element-resolved atomic-scalemicroscopy experiments. By performing imaging for two different viewdirections, we are able to directly measure the in-plane anisotropy of m-GaTeat the sub-Angstrom level, and show that it compares well with the results offirst-principles modeling. Quantum-chemical bonding analyses provide a detailedpicture of the atomic neighbor interactions within the layers, revealing thatvertical Ga-Ga homopolar bonds get stronger when they are distorted androtated, inducing the strong in-plane anisotropy.

Atom-by-Atom Mapping and Understanding of In-Plane Anisotropy in GaTe