Abstract
The results of an electron-spin-resonance investigation of the metastable 4f65d level of Eu2+ in CaF2, SrF2, and BaF2 are presented. The experiments utilized the intense fluorescence from the lowest-lying Γ8(4f65d) level of Eu2+ to the S728(4f7) ground state for the optical detection of resonance transitions in the excited state. The magnitudes of the Zeeman and hyperfine splittings for the excited state are consistent with the model of a large crystal-field splitting for the 5d electron and a considerably smaller coupling of this electron to the 4f6 configuration. The large average g value of 3.80 for this level can be explained by an effective exchange coupling between the 5d spin and the 4f6(FJ7) spin component if this coupling is comparable to the 400-cm1 spin-orbit coupling parameter for the FJ7 multiplets. The anomalous line shapes of the resonance spectrum can be interpreted on the basis of a dynamical Jahn-Teller distortion of the eg orbital of the 5d electron. A singlet tunneling level associated with the Jahn-Teller effect is estimated to be at about 10 cm1 above the orbital doublet Γ8 level in both SrF2 and CaF2 on the basis of the line shapes observed in the resonance spectrum. Previously unidentified optical transitions to these levels have been observed by other workers, who also measured the splitting of the Γ8 level by uniaxial strains and the strain coupling of the singlet tunneling level to the Γ8 level. These piezo-optic data are in quantitative agreement with the model of a dynamical Jahn-Teller interaction for the observed levels. The nature of the fluorescence spectrum of Eu2+ in Ba