An intensive, broad tunable monochromatic Terahertz (THz) emission is generated from S-doped (2 wt. %) GaSe (solid solution GaSe0.91S0.09) crystals by collinear difference frequency generation method. The generated THz signal of 3.8 ns covers the spectral range of 0.57–3.57 THz (84.0–528.0 μm), with a maximal THz output peak power of 21.8 W at 1.62 THz. The THz power conversion efficiency is of 45% higher than that of undoped GaSe, which is mainly contributed to the improved optical properties. The terahertz source is of great potential to be exploited for the out-of-door applications due to the increased crystal hardness.

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