We employ atomically
resolved and element-specific scanning transmission
electron microscopy (STEM) to visualize in situ and
at the atomic scale the crystallization and restructuring processes
of two-dimensional (2D) molybdenum disulfide (MoS2) films.
To this end, we deposit a model heterostructure of thin amorphous
MoS2 films onto freestanding graphene membranes used as
high-resolution STEM supports. Notably, during STEM imaging the energy
input from the scanning electron beam leads to beam-induced crystallization
and restructuring of the amorphous MoS2 into crystalline
MoS2 domains, thereby emulating widely used elevated temperature
MoS2 synthesis and processing conditions. We thereby directly
observe nucleation, growth, crystallization, and restructuring events
in the evolving MoS2 films in situ and
at the atomic scale. Our observations suggest that during MoS2 processing, various MoS2 polymorphs co-evolve
in parallel and that these can dynamically transform into each other.
We further highlight transitions from in-plane to out-of-plane crystallization
of MoS2 layers, give indication of Mo and S diffusion species,
and suggest that, in our system and depending on conditions, MoS2 crystallization can be influenced by a weak MoS2/graphene support epitaxy. Our atomic-scale in situ approach thereby visualizes multiple fundamental processes that
underlie the varied MoS2 morphologies observed in previous ex situ growth and processing work. Our work introduces
a general approach to in situ visualize at the atomic
scale the growth and restructuring mechanisms of 2D transition-metal
dichalcogenides and other 2D materials.