Large-scale fabrication of TMDC is still a challenge to be overcome. Up to now, the most frequently used techniques are either exfoliation of natural layered crystals or the growth via chemical vapor deposition (CVD). Exfoliation is a very time-consuming process with relatively low yield and reproducibility. In CVD, different gaseous precursors decompose on a substrate and react with each other. Thermally evaporated MoO3 and S are commonly used as precursors for the fabrication of MoS2 monolayers via CVD. This technique allows the deposition of monolayered crystallites with a size in the range of micrometers [Dumcenco]. The process is carried out in small experimental reactors, and a uniform deposition on a whole wafer is very challenging. The use of metalorganic precursors is one possibility to enter an industrial scale of fabrication. The development of III/V and II/VI semiconductors has shown that metalorganic chemical vapor deposition (MOCVD) makes controllable and reproducible processes feasible, which are easily scalable and hence suitable for large-area deposition. Additionally, the reactors are well-developed, and a future integration of 2D materials and other semiconductors is within reach. First publications show very good results on the deposition of MoS2 and WSe2 via MOCVD [Kang, Eichfeld]. But despite these works and first simulations of the growth kinetics [Nie], little is known about the growth mechanism. For this reason, we have started to investigate the deposition of 2D MoS2 on an AIXTRON MOCVD reactor.
The experiments are carried out in a horizontal hot-wall MOCVD reactor in a 10 × 2 inch configuration. Molybdenum hexacarbonyl (MCO) and Di-tert-butyl sulfide (DTBS) are used as Mo and S sources, respectively. In preliminary experiments, the carrier gas based transport of the precursors into the reactor and possible growth conditions are tested. Their results are used to develop an initial growth process. This process leads to a uniform, wafer-scale deposition of MoS2 on various substrate types such as sapphire (0001), Si (111), and AlN and GaN templates on sapphire substrates. The deposited films mainly consists of MoS2 bilayers and exhibit a very high initial nucleation density. Further investigations of the influence of the growth temperature, the carrier gas composition and the pretreatment of the substrates are carried out. With optimization of these growth parameters, a crystal growth process closer to thermodynamical equilibrium can be achieved. This results in the formation of triangular crystals on sapphire substrates which are also reported from CVD processes and exhibit higher crystal quality [Dumcenco]. Additional experiments are conducted to investigate the nucleation of the films and to further tune nucleation density and lateral growth rate in order to deposit wafer-scale monolayered MoS2 films.