Giant photon-drag-induced ultrafast photocurrent in diamond for nonlinear photonics

TL;DR

This paper reports a giant photon-drag-induced ultrafast photocurrent in CVD diamond, enabling efficient THz emission for nonlinear photonics, driven by second-order nonlinear effects and photon momentum transfer at grain boundaries.

Contribution

It demonstrates a significant second-order nonlinear photocurrent in diamond via photon drag effect, revealing new mechanisms for THz generation in wide-bandgap semiconductors.

Findings

Giant second-order nonlinear photocurrent observed in CVD diamond.

Distinct roles of circular and linear PDE in THz generation clarified.

CVD diamond exhibits highest THz emission efficiency among carbon allotropes.

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-bandgap 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 {\pi}-{\pi}* transition upon femtosecond laser excitation. Especially, the interplay between circular and linear PDE to the THz generation has been clarified and distinguished under elliptically polarized light excitation. Furthermore, the picosecond ultrafast dynamics of these charge carriers are also verified by the 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.