Abstract
Abstract We have carried out nonlinear spectroscopy by making use of tunable VUV light from synchrotron radiation (SR) together with intense light from a laser. The valence excitons of BaF 2 with a large band gap of ∼11 eV were chosen as our target. A single crystal of BaF 2 was irradiated at 15 K by the two light pulses from the SR (6–9 eV) and an Nd : YAG laser (2.33 eV). Self-trapped exciton luminescence induced by two-photon excitation was detected with a time-gated photon-counting system developed for the present study. This zero-method technique is expected to be sensitive compared to early experiments by an Italian group monitoring transmittance changes. The obtained two-photon spectrum shows a distinct band below the band gap energy. This band includes two contributions, a two-step cascade process and a two-photon absorption process. The energy of the 2 P exciton is estimated to be 10.6 eV at 15 K.
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