Realizing the Intrinsic Anisotropic Growth of 1T′ ReS2 on Selected Au(101) Substrate Toward Large‐Scale Single Crystal Fabrication

Low‐symmetry 2D materials with strong in‐plane anisotropy are ideal platforms for building multifunctional optoelectronic devices. However, the random orientations and easy formation of multidomain structures lead to the single‐crystal synthesis of these materials remains a big challenge. Herein, for the first time, the orientation‐controlled synthesis of ReS2, a typical low‐symmetry 2D material, is explored via interface engineering based on the strong interaction between the material and Au substrates with different symmetries. It is revealed that the lattice orientation and growth behavior of ReS2 are closely relevant to the lattice symmetry of Au facets. Single crystal ReS2 domains with two and even one orientations are acquired on the four‐fold symmetry Au(001) facet and the two‐fold symmetry Au(101) facet, respectively. Combined with density functional theory calculations, it is demonstrated that the synergy of ultra‐strong ReS2‐Au interfacial coupling and reduction of symmetry of Au facet is critical to realizing its intrinsic anisotropic growth. Furthermore, great enhancement of electrical and photoelectrical performances are acquired on the well‐aligned single crystal ReS2 device. The progress achieved in this work provides significant guidance for the controllable synthesis of wafer‐scale single crystals of low‐symmetry 2D materials for their practical device applications.