“…Recently, monoelemental vdW layered materials, such as black phosphorus (BP, Figure 3a), [ 28–33 ] boron, [ 34,35 ] arsenene, [ 36,37 ] tellurium, [ 38,39 ] antimonene, [ 40–43 ] and bismuthine, [ 44,45 ] attract great attentions from researchers. BP stands out among various layered materials due to its modest bandgap, [ 46,47 ] high light absorption, [ 33,48 ] high room‐temperature carrier mobility (≈5000 cm 2 V −1 s −1 ), [ 49–52 ] and nice biological compatibility, [ 53 ] which make it a candidate to apply in various devices, [ 54–56 ] such as photodetector, [ 46,48,57–62 ] ultrafast laser, [ 63–65 ] optical switching, [ 66 ] modulator, [ 67 ] sensor, [ 68 ] and even biomedicine. [ 69–71 ] Intrinsic BP flake possesses a thickness‐dependent direct bandgap from 0.3 eV (bulk) to 2.0 eV (monolayer), corresponding to a maximum photoresponse cutoff wavelength of 4 µm.…”