Spectral profile of the two-photon absorption coefficients in CaF2 and BaF2

Two-photon absorption spectra due to the valence excitons in CaF2 and BaF2 have been measured using the second harmonic of the output of a XeCl-excimer-laser pumped dye laser as a light source. The band gap energies of CaF2 and BaF2 are obtained as 11.8 and 10.6 eV at 298 K, respectively. The two-photon absorption coefficient β in the spectral region below the 2P exciton is expressed by an exponential function of the photon energy in both crystals. The values of β at the 2P exciton peak are about 2×10−9 cm/W for CaF2 and 3×10−9 cm/W for BaF2.