Strong Nonlinearity Induced by Coaxial Alignment of Polar Chain and Dense [BO3] Units in CaZn2(BO3)2

Discovery of new efficient nonlinear optical (NLO) materials with large second-order nonlinearity for the short-wave ultraviolet spectral region (lambda(PM)<= 266 nm, PM=phase-matching) is still very challenging. Herein, a new beryllium-free borate CaZn2(BO3)(2) with Sr2Be2B2O7 (SBBO) double-layered like configuration was rationally designed, which not only preserves the structural merits but also eliminates the limitations of the SBBO crystal. CaZn2(BO3)(2) shows a large PM second harmonic generation (SHG) reponse of 3.8xKDP, which is 38 times higher than that of its barium analogue. This enhancement mainly originates from the (1)[Zn2O6](infinity) polar chains with a large net dipole moment and [BO3] units with a high NLO active density. Our findings show the great significance of the [ZnO4] tetrahedra introduced strategy to design beryllium-free SBBO-type NLO crystals and also verify the feasibility of using simple non-isomorphic substitution to induce giant second-order nonlinearity enhancement.

Automated summary

A new beryllium-free borate CaZn2(BO3)(2) with large second harmonic generation response was designed in this study, demonstrating the significance of designing beryllium-free SBBO-type NLO crystals and the feasibility of inducing giant second-order nonlinearity enhancement through simple non-isomorphic substitution.