Li₂ MTeO₆ (M=Ti, Sn): Mid-Infrared Nonlinear Optical Crystal with Strong Second Harmonic Generation Response and Wide...

Oxide crystals have been widely used in nonlinear optics (NLO) in the ultraviolet-visible and near-infrared regions. Most traditional oxide crystals are restricted to the mid-infrared region due to their narrow transmission window. Hence, attempting to extend infrared cutoff wavelength of oxides has attracted much attention. Herein, we report two new tellurates Li₂ TiTeO₆ (LTT) and Li₂ SnTeO₆ (LST) with broad transparent regions of 0.38-6.72 and 0.38-6.86 μm, respectively, as excellent candidates for mid-infrared NLO applications. Both LTT and LST crystallize in the orthorhombic space group Pnn2. The LTT crystal exhibits intense powder second-order generation efficiency (26×KDP) under the fundamental wavelength of 1064 nm. First-principles calculations and dipole moments were used to illustrate the results of the powder second-harmonic generations based on the crystal structures. Our results provide a novel oxide NLO crystal with a strong SHG and wide transparency range. They also pave a way for the design of new oxide mid-IR NLO crystals.