Phase engineering of two-dimensional (2D) transition metal dichalcogenides (TMDs) such as MoTe2 offers tremendous opportunities in various device applications. However, most of the existing methods so far only address the small-area local phase change or the growth of certain kinds of phases of MoTe2 film by laser irradiation, mechanical strain, or procursor type. Obtaining facile, tunable, reversible, and continuous-phase transition and evolution between different phases in direct growth of large-area, few-layer MoTe2 still remains challenging. Here, we develop a facile method to achieve phase control and transition and report a highly tunable, tellurization velocity-dependent metallic-semiconducting-metallic phase evolution in chemical vapor deposition (CVD) growth of large-area, few-layer MoTe2. We found four different phase stages, including two different types of coexistence phases of both 2H and 1 T' phases, 100% 2H phase, and 100% 1T' phase, would emerge, relying on the adopted tellurization velocity. Importantly, the tellurization velocity should be extremely controlled to obtain 100% 2H phase MoTe2, while 100% 1T' phase requires a fast tellurization velocity. We further found that such metallic-semiconducting-metallic phase evolution took place with a homogeneous spatial distribution and differs from previous reports in which obvious phase separations are usually found during the phase transition. The resulting MoTe2 shows high quality with room-temperature mobility comparable with mechanically exfoliated materials. The results might impact large-scale phase engineering of TMDs and other 2D materials for Weyl semimetal topological physics and potential 2D semiconductor device applications.
Keywords: large-area synthesis; metallic−semiconducting−metallic phase transition; phase engineering; two-dimensional materials.