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Phosphorene, a monolayer of black phosphorus (BP), is an elementaltwo-dimensional material with interesting physical properties, such as highcharge carrier mobility and exotic anisotropic in-plane properties. Tofundamentally understand these various physical properties, it is criticallyimportant to conduct an atomic-scale structural investigation of phosphorene,particularly regarding various defects and preferred edge configurations.However, it has been challenging to investigate mono- and few-layer phosphorenebecause of technical difficulties arising in the preparation of a high-qualitysample and damages induced during the characterization process. Here, wesuccessfully fabricate high-quality monolayer phosphorene using a controlledthinning process with transmission electron microscopy, and subsequentlyperform atomic-resolution imaging. Graphene protection suppresses thee-beam-induced damage to multi-layer BP and one-side graphene protectionfacilitates the layer-by-layer thinning of the samples, rendering high-qualitymonolayer and bilayer regions. We also observe the formation of atomic-scalecrystalline edges predominantly aligned along the zigzag and (101)terminations, which is originated from edge kinetics under e-beam-inducedsputtering process. Our study demonstrates a new method to image and preciselymanipulate the thickness and edge configurations of air-sensitivetwo-dimensional materials.

Fabrication and Imaging of Monolayer Phosphorene with Preferred Edge Configurations via Graphene-Assisted Layer-by-Layer Thinning