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Two-dimensional (2D) crystals' edge structures not only influence theiroverall properties but also dictate their formation due to edge-mediatedsynthesis and etching processes. Edges must be carefully examined because theyoften display complex, unexpected features at the atomic scale, such asreconstruction, functionalization, and uncontrolled contamination. Here, weexamine atomic-scale edge structures and uncover reconstruction behavior inbilayer phosphorene. We use in situ transmission electron microscopy (TEM) ofphosphorene/graphene specimens at elevated temperatures to minimize surfacecontamination and reduce e-beam damage, allowing us to observe intrinsic edgeconfigurations. Bilayer zigzag (ZZ) edge was found the most stable edgeconfiguration under e-beam irradiation. Through first-principles calculationsand TEM image analysis under various tilting and defocus conditions, we findthat bilayer ZZ edges undergo edge reconstruction and so acquire closed,self-passivated edge configurations. The extremely low formation energy of theclosed bilayer ZZ edge and its high stability against e-beam irradiation areconfirmed by first-principles calculations. Moreover, we fabricate bilayerphosphorene nanoribbons with atomically-sharp closed ZZ edges. The identifiedbilayer ZZ edges will aid in the fundamental understanding of the synthesis,degradation, reconstruction, and applications of phosphorene and relatedstructures.

Atomically Sharp, Closed Bilayer Phosphorene Edges by Self-Passivation