Resonant enhancement by a factor of over 20 of direct two-photon absorption from the ground state $^{7}\mathrm{F}_{6}$ to the excited state $^{5}\mathrm{G}_{6}$ of the 4${f}^{8}$ configuration of the ${\mathrm{Tb}}^{3+}$ ion at 40 200 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ has been observed in time-resolved experiments with two separate pulsed lasers. The results provide clear evidence for resonant enhancement of two-photon absorption in rare-earth compounds and imply a similar enhancement for Raman scattering and nonlinear-optical mixing. Two separate contributions to the direct transition moment were observed. When a single laser frequency was used, the intermediate states which made the largest contribution were from excited configurations of opposite parity; those intermediate states were far from resonance. Detailed two-frequency experiments showed, however, that near a single photon $^{7}\mathrm{F}_{6}$${\mathrm{\ensuremath{-}}}^{5}$${\mathrm{D}}_{4}$ resonance, a much stronger contribution arose from the 4${f}^{8}$ configuration $^{5}\mathrm{D}_{4}$ intermediate state. Two-photon absorption was clearly isolated from two-step (incoherent) excitation by varying the timing of two separately triggered lasers.
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