Large-Scale Synthesis of Defect-Free Phosphorene on Nickel Substrates: Enabling Atomistic Thickness Devices.

Addressing the main challenges of defect-free, large-scale synthesis of low-dimensional materials composed of phosphorus atoms is essential for advancing promising phosphorene-based technologies. Using molecular dynamics simulation, we demonstrate the large-scale and defect-free synthesis of phosphorene on Nickel (Ni) substrates. We showed that substrate orientation is crucial in the controllable synthesis of different phosphorene allotropes. Specifically, blue phosphorene was successfully grown on Ni (111) and Ni (100) surfaces, while γ-phosphorene, referred to here as Navy phosphorene, was grown on Ni (110). In addition, temperature control (high temperature) and cooling rate (slow cooling) are also crucial in the formation of P6 hexagons. Finally, we report that the phosphorus pentamers (P5) are the essential precursor for phosphorene synthesis. This work provides a robust framework for understanding and controlling the synthesis of large-area, single-crystalline monolayer phosphorene.