Abstract
The direct calculation of transition line strengths andrelative intensities is presented for two intraconfigurational two-photon absorption (TPA) transitions of Eu3+ in thecubic Cs2NaYF6 host. Crystal field wavefunctions wereutilized for the initial and final fN-electron states andvarious approaches were used in constructing all the 4fN-1 5d1 intermediate-state wavefunctions. The calculatedrelative intensities of the (7F0) Γ1g→(5D2)Γ5g, Γ3gTPA transitions are in reasonable agreement with experiment. Theneglect of J-mixing in the initial state has only a smalleffect upon the calculation, whereas the neglect of spin-orbitcouplings within the initial and terminal states drasticallyreduces the calculated transition linestrengths, but does notmarkedly change the intensity ratios. In the case of the (7F0)Γ1g→(5L6)Γ1g, aΓ5g transitions,serious discrepancies between experiment and theory are foundif the intermediate states are constructed from a 4f5 corecomprising free ion states and the 5d1 crystal fieldstates. Satisfactory agreement is, however, found when the4f5 crystal field states are utilized in constructing theintermediate states. The contributions to the transition momenthave been evaluated for various Hamiltonian terms and theresults are discussed.
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