Giant Photon‐Drag‐Induced Ultrafast Photocurrent in Diamond for Nonlinear Photonics

Abstract Diamond is emerging as an attractive third‐generation wide‐bandgap semiconductor for future on‐chip nonlinear photonics and quantum optics due to its unique thermal, optical, and mechanical properties. However, the light‐driven current under below‐band gap excitation from the second‐order nonlinear optical effect in diamond is still challenging. Herein, a giant second‐order nonlinear photocurrent is observed in the chemical vapor deposition (CVD) diamond by utilizing terahertz (THz) emission spectroscopy. This ultrafast photocurrent originates from the photon drag effect (PDE), during which the momentum transfer from the incident photons to the charge carriers at the rich grain boundaries of the CVD diamond after the exclusive subgap π–π * transition upon femtosecond laser excitation. Especially, the interplay between circular and linear PDE to the THz generation is clarified and distinguished under elliptically polarized light excitation. Furthermore, the picosecond ultrafast dynamics of these charge carriers are also verified by infrared spectroscopy. Owing to the giant photon‐drag‐induced ultrafast photocurrent, the CVD diamond presents the highest THz emission efficiency compared with the reported carbon allotropes, which expands the new functionality of diamond nonlinear photonics into on‐chip THz devices.