Intrinsic correlation between electronic structure and degradation: from few layers to bulk black phosphorus

Black phosphorus (BP) has received much attention due to its fascinating properties, such as a high mobility and tunable band gap which covers the band gap lacuna between graphene and transition metal dichalcogenides. However, these advantages have been overshadowed due to the fast degradation of BP in ambient conditions. To overcome this obstacle, the degradation mechanisms should be unveiled with direct observation followed by a thorough analysis. Here, we reveal two sequential degradation processes and layer‐dependent degradation rates of BP under dark conditions by scanning Kelvin probe microscopy measurements and theoretical modeling. The layer‐dependent degradation is successfully interpreted with the oxidation model based on the Marcus‐Gerischer theory. Under dark conditions, the electron transfer rate from BP to oxygen molecule depends on the number of layers that give different carrier concentrations. The oxidation rate is strongly dependent on the number of layers, and thus carrier concentrations. This suggests the possibility of stability improvement by carrier modulation. This work not only provides a deeper understanding of the degradation mechanism itself but also suggest new strategies for stable BP‐based electronics design.

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