Herein, a novel IR NLO oxytelluride SrGeOTe was successfully designed and synthesized through a "partial O-to-Te substitution" strategy. Compared with the parent oxide, SrGeOTe not only successfully achieves a phase-matchability transition (from NPM to PM), but also greatly improves the linear and NLO performances, including a wide band gap (2.26 eV), strong SHG response (1.3 × AgGaSe) and large optical anisotropy (Δ = 0.152@2090 nm). The analyses of the structure-property relationship and SHG-density indicate that the bridging oxygen in the [OGe-O-GeTe] prism unit plays the most important role in the multiplication SHG effect. This work provides some insights into the design and exploration of novel IR NLO materials.
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