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Molecular Construction from AgGaS2 to CuZnPS4: Defect-Induced Second Harmonic Generation Enhancement and Cosubstitution-Driven Band Gap Enlargement
journal contribution
posted on 2020-03-17, 14:44 authored by Zhuang Li, Shengzi Zhang, Zhiwei Huang, Li-Dong Zhao, Ece Uykur, Wenhao Xing, Zheshuai Lin, Jiyong Yao, Yicheng WuHerein, we offer
a simple but crucial case for rational design
and syntheses of infrared nonlinear optical (NLO) materials by employing
state-of-the-art AgGaS2 as a parent model. On the basis
of inheriting structural advantages of AgGaS2, an as-grown
CuZnPS4 crystal exhibits a sharply enlarged energy gap
(3.0 eV) benefiting from the cosubstitution of Ag with lighter Cu/Zn.
Remarkably, the valence electron distribution of CuZnPS4 is optimized by bringing in cation vacancy defects, which significantly
reinforce the second harmonic generation (SHG) (3 × AgGaS2) and compensate for the adverse effect of band gap enlargement.
Careful experimental and theoretical investigations illustrate that
CuZnPS4 strikes a desirable balance among a strong SHG
response, good phase matchability, large band gap, high laser damage
threshold, outstanding physicochemical stability, low melting point,
and cost-effective but non-toxic composition, which might shed light
on follow-up design and exploratory synthesis of NLO materials.