Exploring Deep-UV Nonlinear Optical Materials with Enhanced Second Harmonic Generation Response and Birefringence in Fluoroaluminoborate Crystals

Deep-UV (DUV) nonlinear optical (NLO) materials are of vital importance to demanding DUV laser applications; however, those with a large NLO coefficient, wide band gap, and sufficient phase-matching ability are rare. In this work, by combining π-conjugated B3O6 groups and distort AlO3F tetrahedra, we successfully designed and synthesized two fluoroaluminoborates, RbAlB3O6F (RABF) and Cs0.5Rb0.5AlB3O6F (CRABF). In addition, the solid solution CsxRb1–xAlB3O6F (0.2 x 3O6 and AlO3F groups contribute to the SHG responses. Remarkably, it also indicates that RABF exhibits a large birefringence (Δn = 0.0946 at 1064 nm), which is capable of realizing deep-UV phase matching down to 174 nm. The exploration of fluoroaluminoborates provides a new perspective for searching excellent deep-UV NLO materials.