Three-in-One Strategy Constructing a Series of Hybrid Tetrahedral Motif-Based Selenides with Balanced Second-Order Nonlinear Optical Performance

Concurrently achieving suitable second harmonic generation (SHG) effect and high laser-induced damage threshold (LIDT) is challenging for infrared nonlinear optical (NLO) materials. Here, a series of pentanary infrared NLO materials (CsMMSnSe6)-M-III-Sn-IV (M-III = Ga, In; M-IV = Si, Ge) have been obtained by a three-in-one strategy, viz. three kinds of elements (M-III, M-IV, and Sn) in one position, which is first adopted to design NLO materials. Their three-dimensional structures are constructed by the MQ(4) (M denotes M-III, M-IV, and Sn) tetrahedral units. They exhibit promising hybrid NLO properties, witnessed by their moderate/large SHG effects of 0.52, 0.98, 1.05, and 1.12 x AgGaS2, and high powder LIDT values of 6.9, 4.1, 8.1, and 5.4 x AgGaS2, respectively. These NLO properties are well verified by the DFT calculation results. The three-in-one strategy of designing high-performance infrared NLO materials will stimulate more investigations in this field.

Automated summary

The pentanary infrared NLO materials achieved suitable SHG effects and high LIDT values through a three-in-one design strategy. They exhibit promising NLO properties, which will stimulate further investigations in this field.