Hg-based chalcogenides possess diverse structures, large nonlinear-optical (NLO) responses, and suitable birefringences, making them potentially suitable for numerous crucial criteria of practical application as infrared (IR) NLO crystals. Here, a new pentanary Hg-based sulfide KBaHgInS has been discovered by a high-temperature solid-state method. It crystallizes in the orthorhombic 222 space group, and its one-dimensional structure is constructed by {[InS]} chains and isolated [HgS] planar quadrilateral units located bewteeen the chains, representing a novel type of chalcogenide. KBaHgInS exhibits a moderate NLO effect of 0.5 × AGS at 2.1 μm and a high laser-induced damage threshold of ∼5.8 × AGS, as well as a band gap of 2.98 eV, demonstrating that KBaHgInS is a potential IR NLO material. This work enriches the structural chemistry of chalcogenides and the family of Hg-based IR NLO chalcogenides.
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