SrHgGeOS: A Hg-Based Oxychalcogenide Infrared Nonlinear Optical Material Exhibiting Favorable Balance between a Large Band Gap and Strong Second Harmonic Generation Response.

Currently, oxychalcogenides with mixed-anion groups that integrate the property advantages of oxides (wide optical band gap) and chalcogenides [strong second harmonic generation (SHG) response] through chemical substitution engineering have attracted widespread interest and are considered to be important candidates for infrared (IR) nonlinear optical (NLO) materials. Herein, the first Hg-based oxychalcogenide SrHgGeOS with mixed anion [GeOS] units has been successfully synthesized through a spontaneous crystallization method, which exhibits a favorable balance between the strong SHG response (0.7 × AgGaS) and large optical band gap (2.9 eV). In addition, SrHgGeOS shows high laser-induced damage threshold (LIDT, 2.1 × AgGaS) as well as phase-matching (PM) performance. Theoretical calculations indicate that the SrHgGeOS encompasses large birefringence of 0.128@2090 nm (3.3 × AgGaS) and its SHG density mainly comes from [HgS] tetrahedra and [GeOS] units. This work not only demonstrates that SrHgGeOS is a promising IR NLO material but also provides new ideas for the exploration of Hg-based oxychalcogenide IR NLO materials.