UV-induced two-photon absorption in BiB3O6 single crystals

We show that BiB₃O₆ (BiBO) crystals, well known for their excellent second harmonic generation (SHG) properties, may also be of interest for third-order optical phenomena, particularly for two-photon absorption (TPA). Photoinduced TPA measurements were performed under illumination of excimer Xe–F laser (λ = 217 nm) as a photoinducing (pumping) beam. It created a thin surface layer (about 85 nm) that was a source of the observed photoinduced TPA. Raman shifted Nd-YAG laser radiation (λ = 1.9 μm) as well as its second and fourth harmonics (λ = 950 and λ = 475 nm, respectively) were used as fundamental (probing) beams of the TPA. The highest values of the TPA β coefficient were achieved for a polarization of the pumping light directed along crystallographic axis b. Quantum chemical simulations indicate on substantial contribution of UV-induced electron–phonon anharmonicity to the observed TPA. The obtained values of TPA coefficients indicate a possibility of using BiBO crystals as UV-operated optical limiters in a wide spectral range.