Strong-field nonlinear optical properties of monolayer black phosphorus

Within the past few years, atomically thin black phosphorus (BP) has been demonstrated as a fascinating new 2D material that is promising for novel nanoelectronic and nanophotonic applications, due to its many unique properties such as a direct and widely tunable bandgap, high carrier mobility and remarkable intrinsic in-plane anisotropy. However, its important extreme nonlinear behavior and the ultrafast dynamics of carriers under strong-field excitation have yet to be revealed. Herein, we report nonperturbative high harmonic generation (HHG) in monolayer BP by first-principles simulations. We show that BP exhibits extraordinary HHG properties, with clear advantages over three major types of 2D materials under intensive study, i.e., semimetallic graphene, semiconducting MoS₂, and insulating hexagonal boron nitride, in terms of HHG cutoff energy and spectral intensity. This study advances the scope of current research activities on BP into a new regime, suggesting its promising future in the applications of extreme-ultraviolet and attosecond nanophotonics and also opening doors to investigate the strong-field and ultrafast carrier dynamics of this emerging material.