Hg3P2S8: A New Promising Infrared Nonlinear Optical Material with a Large Second-Harmonic Generation and a High Laser-Induced Damage Threshold
The development of new infrared (IR) nonlinear optical (NLO) materials with strong second-harmonic generation (SHG) responses and high laser-induced damage thresholds (LIDTs) is urgent but challenging. Herein, the defective diamond-like chalcogenide Hg3P2S8 (HPS) was rationally designed and fabricated by a flexible and rigid tetrahedral motif combined strategy. HPS exhibits a phase-matching SHG response of ∼3.6 × AGS (the largest one in the reported ternary sulfides), high LIDT (∼3 × AGS), wide IR transparent region (0.43–16.3 μm), moderate birefringence (0.043 at 1064 nm), and good physicochemical stability and crystal growth habits. Theoretical analyses confirm that the large SHG effect originates from the synergistic effects between distorted HgS4, PS4, and vacancy-induced nonbonding electrons. The results indicate that HPS is a promising NLO candidate for high-power, high-efficiency laser output in the mid-IR region, which provides an insight into the exploration of new IR NLO materials.
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