Claudia Bock

To implement 2D molybdenum disulfide (MoS 2 ) in the flexible electronic industry, large, uniform, and crystalline films on flexible substrates are needed. Thermal atomic layer deposition (ALD) generates large‐area uniform MoS 2 films at low temperatures directly on temperature‐sensitive substrates. But if the grown films are amorphous, a high‐temperature posttreatment of the whole sample, which may cause thermal degradation of the substrate or other layers, needs to be avoided. In this article, the crystallization of amorphous MoS 2 layers deposited by thermal ALD processed with picosecond laser pulses ( λ = 532 nm), in a “cold” annealing process, is reported. The laser fluence range varies from = 8.73 mJ cm −2 to = 18.25 mJ cm −2 with scanning speeds from = 240 mm s −1 to = 2640 mm s −1 . The crystallization and the influence of the processing parameters on the film morphology are analyzed in detail by Raman spectroscopy and scanning electron microscopy. Furthermore, a transition of amorphous MoS 2 by laser annealing to self‐organized patterns is demonstrated and a possible process mechanism for the ultrashort‐pulsed (usp)‐laser annealing is discussed. Finally, the usp laser annealed films are compared to thermally and continuous‐wave‐laser‐annealed samples.