Sr 2 HgGe 2 OS 6 : 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 Sr 2 HgGe 2 OS 6 with mixed anion [GeOS 3 ] units has been successfully synthesized through a spontaneous crystallization method, which exhibits a favorable balance between the strong SHG response (0.7 × AgGaS 2 ) and large optical band gap (2.9 eV). In addition, Sr 2 HgGe 2 OS 6 shows high laser-induced damage threshold (LIDT, 2.1 × AgGaS 2 ) as well as phase-matching (PM) performance. Theoretical calculations indicate that the Sr 2 HgGe 2 OS 6 encompasses large birefringence of 0.128@2090 nm (3.3 × AgGaS 2 ) and its SHG density mainly comes from [HgS 4 ] tetrahedra and [GeOS 3 ] units. This work not only demonstrates that Sr 2 HgGe 2 OS 6 is a promising IR NLO material but also provides new ideas for the exploration of Hg-based oxychalcogenide IR NLO materials.