Uncovering a Vital Band Gap Mechanism of Pnictides.

ABSTRACT: Pnictides are superior infrared (IR) nonlinear optical (NLO) material candidates, but the exploration of NLO pnictides is still tardy due to lack of rational material design strategies. An in-depth understanding structure-performance relationship is urgent for designing novel and eminent pnictide NLO materials. Herein, this work unravels a vital band gap mechanism of pnictides, namely P atom with low coordination numbers (2 CN) will cause the decrease of band gap due to the delocalization of non-bonding electron pairs. Accordingly, a general design paradigm for NLO pnictides, ionicity-covalency-metallicity regulation is proposed for designing wide-band gap NLO pnictides with maintained SHG effect. Driven by this idea, millimeter-level crystals of MgSiP2 are synthesized with a wide band gap (2.34 eV), a strong NLO performance (3.5 x AgGaS₂ ), and a wide IR transparency range (0.53-10.3 µm). This work provides an essential guidance for the future design and synthesis of NLO pnictides, and also opens a new perspective at Zintl chemistry important for other material fields.

SUBMITTER: Chen J 

PROVIDER: S-EPMC9109059 | biostudies-literature | 2022 May

REPOSITORIES: biostudies-literature