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SrZnGeS4: A Dual-Waveband Nonlinear Material With A Transparency Spanning UV-Vis and Far-IR Spectral Regions.

Non-linear optical chalcogenides with a wide band gap (Eg) and excellent NLO properties are key materials for highly desirable multiwaveband tunable optical parametric oscillators (OPOs). We exploit the "electronic structure engineer bucket effect" to develop a novel dual-waveband SrZnGeS4 with an ultrawide transparency window. It exhibits an asymmetric Fdd2 structure that consists of layers formed by corner-sharing [ZnGeS6] dimers. SrZnGeS4 is transparent from 0.30 to 23.6 μm, spanning the UV-, vis-, mid- and far-IR spectral regions and has the widest Eg (3.63 eV) in the AeMIIMIVQ4 family to date. It exhibits phase matching, high SHG intensities (e.g., 11.0 × KDP and 17.5 × AGS under λinc = 1450 and 950 nm, respectively), and a very high laser-induced damage threshold (35 × AGS). These results not only suggest bright prospects for high-power laser applications but may also enable applications of the multiwaveband OPO system from the UV-visible to far-IR regions.