Deeply Exploring Anisotropic Evolution toward Large-Scale Growth of Monolayer ReS₂

Among large numbers of transition metal dichalcogenides (TMDCs), monolayer rhenium disulfide (ReS₂) is of particular interest due to its unique structural anisotropy, which opens up unprecedented opportunities in dichroic atomical electronics. Understanding the domain structure and controlling the anisotropic evolution of ReS₂ during the growth is considered critical for increasing the domain size toward a large-scale growth of monolayer ReS₂. Herein, by employing angle-resolved Raman spectroscopy, we reveal that the hexagonal ReS₂ domain is constructed by six well-defined subdomains with each b-axis parallel to the diagonal of the hexagon. By further combining the first-principles calculations and the transmission electron microscopy (TEM) characterization, a dislocation-involved anisotropic evolution is proposed to explain the formation of the domain structures and understand the limitation of the domain size. Based on these findings, growth rates of different crystal planes are well controlled to enlarge the domain size, and moreover, single-crystal domains with a triangle shape are obtained. With the improved domain size, large-scale uniform, strictly monolayer ReS₂ films are grown further. Scalable field-effect transistor (FET) arrays are constructed, which show good electrical performances comparable or even superior to that of the single domains reported at room temperature. This work not only sheds light on comprehending the novel growth mechanism of ReS₂ but also offers a robust and controllable strategy for the synthesis of large-area and high-quality two-dimensional materials with low structural symmetry.