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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 (MoS 2 ) films. To this end, we deposit a model heterostructure of thin amorphous MoS 2 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 MoS 2 into crystalline MoS 2 domains, thereby emulating widely used elevated temperature MoS 2 synthesis and processing conditions. We thereby directly observe nucleation, growth, crystallization, and restructuring events in the evolving MoS 2 films in situ and at the atomic scale. Our observations suggest that during MoS 2 processing, various MoS 2 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 MoS 2 layers, give indication of Mo and S diffusion species, and suggest that, in our system and depending on conditions, MoS 2 crystallization can be influenced by a weak MoS 2 /graphene support epitaxy. Our atomic-scale in situ approach thereby visualizes multiple fundamental processes that underlie the varied MoS 2 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.

Atomic-Scale in Situ Observations of Crystallization and Restructuring Processes in Two-Dimensional MoS2 Films

Atomic-Scale in Situ Observations of Crystallization and Restructuring Processes in Two-Dimensional MoS₂ Films