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Two-dimensional (2D) transition metal dichalcogenides (TMDCs) have been thesubject of sustained research interest due to their extraordinary electronicand optical properties. They also exhibit a wide range of structural phasesbecause of the different orientations that the atoms can have within a singlelayer, or due to the ways that different layers can stack. Here we report thefirst study of direct-visualization of structural transformations inatomically-thin layers under highly non-equilibrium thermodynamic conditions.We probe these transformations at the atomic scale using real-time, aberrationcorrected scanning transmission electron microscopy and observe strongdependence of the resulting structures and phases on both heating rate andtemperature. A fast heating rate (25 C/sec) yields highly ordered crystallinehexagonal islands of sizes of less than 20 nm which are composed of a mixtureof 2H and 3R phases. However, a slow heating rate (25 C/min) yieldsnanocrystalline and sub-stoichiometric amorphous regions. These differences areexplained by different rates of sulfur evaporation and redeposition. The use ofnon-equilibrium heating rates to achieve highly crystalline andquantum-confined features from 2D atomic layers present a new route tosynthesize atomically-thin, laterally confined nanostrucutres and opens newavenues for investigating fundamental electronic phenomena in confineddimensions.

Direct Visualisation of Out-of-Equilibrium Structural Transformations in Atomically-Thin Chalcogenides