Large second-harmonic generation (SHG) response and broad band gap are two important and competitive parameters. It is difficult to balance them out in one material. In this work, by coupling alkali earth metal (AEM) octahedra with large highest occupied molecular orbital (HOMO)-lowest unoccupied molecular orbital (LUMO) gap and nonlinear optical (NLO)-active tetrahedra units, nine noncentrosymmetric (NCS) compounds, belonging to a new quaternary chalcogenide family ABCQ with unique windmill-like [MgMQ] (M = Al, Ga; Q = S, Se) units constructed by alternated [MgQ] octahedra and [MQ] tetrahedra, are rationally designed and fabricated. The compounds show a stable structural framework but adjustable optical properties. Among them, NaMgGaSe shows a large SHG response (∼1 × AgGaS (AGS)), wide band gap (in selenide) (2.77 eV), high laser-induced damage threshold (LIDT) (∼2.3 × AGS), and suitable birefringence (0.079@546 nm). It should be a potential candidate for infrared (IR) nonlinear optical (NLO) materials. The results enrich the chemical diversity of chalcogenides and open an avenue for the development of new IR NLO materials through the octahedra and tetrahedra coupled strategy.
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