Vertically stacked two-dimensional
(2D) transition-metal dichalcogenide
(TMDC) heterostructures (HSs) offer a prospective approach to manipulating
their physical characteristics via a transfer strategy. However, the
synthesis of 2D multilayered TMDC vertical HSs is still challenging
through one-step chemical vapor deposition (CVD). Here, two-, three-,
and four-layer 2D TMDC van der Waals (vdW) HSs, including 1L-MoS2/1L-WS2, 1L-WS2/1L-MoS2,
1L-MoS2/2L-WS2, 2L-MoS2/2L-WS2, and 3L-MoS2/1L-WS2, have been achieved
under two opposite preparation routes through a one-step CVD approach
via alternating utilization of metallic Mo (or W) foil and WO3 (or MoO3) powder as precursors. The structure,
phase number, and layer number of these peculiar multilayered HSs
are comprehensively evaluated by optical microscopy, atomic force
microscopy, and Raman and photoluminescence spectroscopy/mapping.
Our results suggest that the growth of these multilayered vdW HSs
may be attributed to the characteristic difference between metallic
Mo (or W) foil and MoO3 (or WO3) powder and
the effect of the growth temperature on the concentration evolution
of Mo/W atoms in vapor, and the reaction with S vapor. Moreover, the
new growth strategy for the fabrication of multilayered vertical HSs
offers a novel and innovative method for the application of multilayered
HSs to diverse fields, including photodetectors, catalysts, and solar
cells.