The direct calculation of transition line strengths and
relative intensities is presented for two intraconfigurational
two-photon absorption (TPA) transitions of Eu3+ in the
cubic Cs2NaYF6 host. Crystal field wavefunctions were
utilized for the initial and final fN-electron states and
various approaches were used in constructing all the 4fN-1 5d1 intermediate-state wavefunctions. The calculated
relative intensities of the (7F0) Γ1g→(5D2)Γ5g, Γ3g
TPA transitions are in reasonable agreement with experiment. The
neglect of J-mixing in the initial state has only a small
effect upon the calculation, whereas the neglect of spin-orbit
couplings within the initial and terminal states drastically
reduces the calculated transition linestrengths, but does not
markedly change the intensity ratios. In the case of the
(7F0)Γ1g→(5L6)Γ1g,
aΓ5g transitions,
serious discrepancies between experiment and theory are found
if the intermediate states are constructed from a 4f5 core
comprising free ion states and the 5d1 crystal field
states. Satisfactory agreement is, however, found when the
4f5 crystal field states are utilized in constructing the
intermediate states. The contributions to the transition moment
have been evaluated for various Hamiltonian terms and the
results are discussed.