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Over decades, guided by the anionic group theory, the majority work has beenfocused on the anionic-moiety of a nonlinear optical material, however, theproperty guided structure modification and design on the cationic-moiety haslong been neglected. Herein, we report for the first time a coordinationstrategy on the cationic-moiety, as demonstrated by the first exmple,[Ag(NH3)2]2SO4 vs Ag2SO4, the coordination of the plus one Ag+ cation by theneutral ligand forming the [Ag(NH3)2]+ cationic-moiety drives the formation ofthe noncentrosymmetric tetragonal P-421c structure which exhibits a remarkableproperty improvement, including a strong SHG intersity (1.4*KDP vs 0 @1064 nm),and a large birefringence (delta(n)cal.: 0.102 vs 0.012 @1064 nm). Furthermore,we discover that owing to the strong hydrogen bonds and spatial confinement of[SO4]2- anions, the cation [Ag(NH3)2]+ bends parallel to the crystallographic caxis with a bond angle of N-Ag-N = 174.35deg, generating a permenant dipolemoment z = -0.12 D that is responsible for the large birefringence thatenlarges the range of the phase matching SHG laser output. We believe what wediscover is only a glimpse of the long been neglected crystal engineering onthe cationic-moiety. Encourage by this work, exciting works on other ioniccompound systems shall flood in.

[Ag(NH3)2]2SO4: A coordination strategy on the cationic-moiety to design nonlinear optical materials