Two novel nonlinear optical carbonates in the deep-ultraviolet region: KBeCO(3)F and RbAlCO(3)F(2)

With the rapid developments of the all-solid-state deep-ultraviolet (deep-UV) lasers, the good nonlinear optical (NLO) crystal applied in this spectral region is currently lacking. Here, we design two novel NLO carbonates KBeCO(3)F and RbAlCO(3)F(2) from the first-principles theory implemented in the molecular engineering expert system especially for NLO crystals. Both structurally stable crystals possess very large energy band gaps and optical anisotropy, so they would become the very promising deep-UV NLO crystals alternative to KBBF. Recent experimental results on MNCO(3)F (M = K, Rb, Cs; N = Ca, Sr, Ba) not only confirm our calculations, but also suggest that the synthesis of the KBeCO(3)F and RbAlCO(3)F(2) crystals is feasible.