Infrared nonlinear optical performances of a new sulfide β-PbGa2S4
Nonlinear optical (NLO) crystals can produce tunable lasers through the direct second-harmonic generation (SHG) process, which is of great significance in modern laser technology. Herein, a new chalcogenide β -PbGa 2 S 4 ( 1 ) crystallized in space group of Pna 2 1 was synthesized via high-temperature solid-state reactions. Compound 1 is composed of a three-dimensional framework [Ga 8 S 16 ] 8− with hexagonal voids filled by Pb atoms via covalent Pb–S interactions. Importantly, it exhibits promising NLO performances, such as phase-matchable SHG efficiency (0.6×AgGaS 2 @1200 nm and 0.1×AgGaS 2 @1910 nm), moderate band-gap (2.46 eV), suitable laser-induced damage threshold (3.0×AgGaS 2 ), and a broad IR transparency window (0.5–25.0 µm). SHG response of 1 is mainly attributable to the occupied S–3p and Ga–4p states and unoccupied S–3p and Pb–6p states.
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