Infrared (IR) nonlinear optical (NLO) crystals are the major materials to widen the output range of solid-state lasers to mid-infrared regions, but they are still inadequate for application due to… Click to show full abstract
Infrared (IR) nonlinear optical (NLO) crystals are the major materials to widen the output range of solid-state lasers to mid-infrared regions, but they are still inadequate for application due to the difficulties in balancing the large band gaps and strong NLO response. The diamond-like structure is a potential structural template to explore IR NLO materials. Herein, a computational workflow is proposed for exploring compounds with diamond-like structures, a series of LiMgGaSe3 structures were predicted successfully through this workflow, and LiMgGaSe3-I-III exhibited good optical performances in a large band gap (2.75-2.92 eV), strong SHG response (1.2-1.3 × AGS), and suitable birefringence (0.0470-0.0783 at 1064 nm). The in-depth mechanism explorations strongly demonstrate that the synergistic effect of alkaline earth metal tetrahedral [MgSe4] and [GaSe4] units is the main origin of large SHG response. The foregoing results suggest that our workflow can accelerate the discovery of new mid-IR NLO materials with diamond-like structures.
               
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