Some
of the distinct optical, catalytical, and electronic properties
of few-layer MoS2 films arise from a specific orientation
of the MoS2 layers. The growth of horizontally or vertically
aligned MoS2 during the sulfurization of predeposited Mo
film can be controlled by various physical conditions such as temperature,
heating rate, Mo film thickness, or sulfur vapor pressure. However,
due to the inherent limitations of performing real-time and in situ experiments during sulfurization in a standard growth
chamber, only a limited number of analytical techniques can be used
to elucidate the in-process phase transformation. Here, we present
a comprehensive real-time study of the growth of few-layer MoS2 films by sulfurization of Mo films using in situ grazing-incidence wide-angle X-ray scattering. We demonstrate that
the process gas flow, and thus the sulfur partial vapor pressure,
is the key control parameter for the few-layer MoS2 layer
orientation while all other process parameters remain fixed. Tracking
the crystallization of few-layer MoS2 layers in real-time
allowed us to estimate the activation energy required for both horizontal
and vertical orientations. Growth of either horizontal or vertical
MoS2 was observed without a metastable transition between
them throughout the sulfurization.