Design of the Ionic Organic Nonlinear Optical Material NH4[LiC3H(CH3)O4] with Ultrawide Band Gap and Moderate Birefringence

Ionic organic crystals containing organic planar p-conjugated units has become one of the hot spots as nonlinear optical (NLO) materials. However, although this type of ionic organic NLO crystals commonly have remarkable second harmonic generation (SHG) responses, they also suffer from overlarge birefringences and relatively small band gaps that be hardly beyond 6.2 eV. Herein, a flexible p-conjugated [C3H(CH3)O-4](2-) unit was theoretically revealed, showing great potential for designing NLO crystals with balanced optical properties. Accordingly, through the reasonable NLO-favourable layered design, a new ionic organic material, NH4[LiC3H(CH3)O-4], was successfully obtained. As expected, it achieves not only a large SHG effect (4xKDP), but also a suitable birefringence (0.06@546 nm) and an ultrawide band gap (>6.5 eV). This study provides a new flexible p-conjugated NLO-active unit, contributing to design more ionic organic NLO materials with excellent balanced optical properties.

Automated summary

Ionic organic crystals with organic planar p-conjugated units are popular as nonlinear optical (NLO) materials. However, these crystals often have large birefringences and small band gaps. A new flexible p-conjugated unit, [C3H(CH3)O-4](2-), was theoretically revealed to have balanced optical properties. By designing a new NLO-favourable structure, a new ionic organic material, NH4[LiC3H(CH3)O-4], was obtained with a large SHG effect, suitable birefringence, and ultrawide band gap. This study contributes to the design of more NLO materials with balanced optical properties.