Moreover, BP has a 0.3-1.5 eV thicknessdependent direct bandgap [27,28] ranging from the mid-infrared to visible region, supplying the bandgap interspace between monolayer graphene (below 0.2 eV) and TMDCs (1-2.5 eV). [3,29] With high carrier mobility (≈10 3 cm 2 V −1 s −1), [4,30] BP has also been viewed as a promising candidate for the fabrication of field-effect transistors and photodetectors. [11,31-34] While BP is being considered for long-term applications owing to its high performance, its terrible preservation in air hampers practical application. After exposing mechanically exfoliated flakes to oxygen or water vapor under ambient conditions, rapid degradation takes place in a very short timescale (minutes), [35,36] greatly impacting the benign nature of the material. Until now, there have been many reports on quantum dots and nanosheets in BP dispersions through the liquidphase exfoliation technique. [10,37-40] Nevertheless, it is difficult to guarantee the stable value of relevant tests because of the metastable BP products that are completely in an organic solvent environment and of indefinitely small size. Another way to improve the antioxidant capacity of BP is the doping approach. Particularly, doping engineering [41] including substitution doping, intercalation doping, surface charge transfer doping, and electrostatic carrier doping, has been demonstrated to be an easy but pragmatic technique for the amelioration of the physicochemical properties of BP. [41] Substitution doping with S, Se, and Te provides extra freedom with controllable characteristics. [42-45] However, the doping function of these elements on nonlinear optical properties [46-50] or ultrafast photonic applications [51-55] has been minimally explored so far. Selenium-doped BP (Se-BP), synthesized by the chemical vapor transport method, is reported to exhibit some intriguing characteristics. [44,56,57] Previous studies have found that Se doping renders BP enhanced long-term air stability and an optical response ascribed to the regulation of intrinsic carrier density. [56] Under a doping range of 0-1.6%, Se atoms effectively reduce the probability of phosphine oxidation by decreasing the conduction band close to or even lower than the redox potential of O 2 /O , 2 − which allows BP to achieve air stability that lasts for several days. [44] The high-quality crystal structure of Se-BP coincides with that of BP, which is convenient for dissociation and peeling off, resulting in good bipolar electrical