Pulsed laser interactions provide unique, highly nonequilibrium conditions for synthesis and processing of new materials, enabling access to metastable phases and nanostructures that can be explored by pulsed laser ablation (PLA), pulsed laser deposition (PLD), and laser processing. Current demands for quantum materials require understanding of the structure and properties at the atomic-level to reveal defects and their correlated properties. Atomically-thin 2D layered materials (such as graphene, MoS2 and other transition metal dichalcogenides (TMDs)) and their heterostructures – formed by stacking layers in different orientations – form a tunable palette of materials that are synthesizable, computationally tractable, and can be atomistically characterized. Here, we describe progress in both the implementation and automation of real-time in situ diagnostics during PLD and laser processing to reveal the synthesis pathways and metastable states of atomically-thin 2D materials as they grow, and advance efforts towards their autonomous synthesis.
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