Layer Tunable Third-Harmonic Generation in Multilayer Black Phosphorus

Black phosphorus has been the subject of growing interest due to its unique band structure that is both layer dependent and anisotropic. While many have studied the linear optical response of black phosphorus, the nonlinear response has remained relatively unexplored. Here we report on the observation of third-harmonic generation in black phosphorus using an ultrafast near-IR laser and measure Chi(3) experimentally for the first time. It was found that the third-harmonic emission is highly anisotropic, dependent on the incident polarization, and varies strongly with the number of layers present due to signal depletion and phase-matching conditions.