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Physical Review B

Two-Photon Excitation of the 4f{sup 1} --> 5d{sup 1} Transitions of Ce{sup3+} in LuPO{sub 4} and YPO{sub 4}

Joost Sytsma, David Piehler, Norman M. Edelstein, L. A. Boatner, M. M. Abraham

Published Feb 1, 1993• 0 citations
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Abstract

Two-photon excitation (TPE) spectra of the 4f 1 -?5d 1 transitions of Ce 3 + in LuP0 4 and YP0 4 have been investigated.For Ce3+ in LuP04, transitions to four out of the five 5d 1 levels are observed as zero-phonon lines.The symmetry properties of the levels were obtained from the polarization dependence of the TPE signals.Measurements on Ce 3 + inYP0 4 support the given assignments.Although a crystal-field fit yields a satisfactory RMS energy deviation, an unrealistic value of the spin-orbit coupling parameter, ( 5 d1, is obtained.The • vibronic coupling appears to be smaller than for the single-photon absorption spectra, and the vibronic bands show a rich structure.There are striking differences between the energies and the relative intensities of the vibronic lines and the associated zero-phonon lines.The vibronic coupling is also found to be strongly dependent on the Ce 3 + concentration.78.50.Ec,42.65.-k

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The observation of two-photon absorption by a very efficient up-converted emission is reported for ${\mathrm{Ho}}^{3+}$ in Ca${\mathrm{F}}_{2}$, Sr${\mathrm{F}}_{2}$, and Cd${\mathrm{F}}_{2}$ with both cw- and pulse-laser excitations. The two-photon excitation spectra are found to be highly structured and consist of two bands: The band $A$ is excited by the dye-laser photons of frequencies 15 400-15 700 ${\mathrm{cm}}^{\ensuremath{-}1}$: The band $B$ is excited by the dye-laser photons of frequencies 15 800-16 400 ${\mathrm{cm}}^{\ensuremath{-}1}$. No one-photon absorption is observed for ${\mathrm{Ho}}^{3+}$ in the above lattices at twice these frequencies. Studies of concentration dependence, temperature dependence, and dependence on the pulse repetition rate are used for the assignment of the band. The investigation shows that the two bands $A$ and $B$ arise from two different modes of two-photon excitation. The band $A$ is assigned to arise from a sequential (stepwise) two-photon excitation $^{5}I_{8}\ensuremath{\rightarrow}^{5}F_{5}\ensuremath{\rightarrow}^{5}D_{2}$. The band $B$ is assigned to arise from the direct two-photon absorption $^{5}I_{8}\ensuremath{\rightarrow}^{3}L_{8}$. Our results are in agreement with the prediction of the Judd-Ofelt theory of lanthanide transition intensities.

Physical review. B, Condensed matter•Jul 1, 1983•22 citations
Two-photon excitation (TPE) spectra of the 4f 1 -?5d 1 transitions of Ce 3 + in LuP0 4 and YP0 4 have been investigated.For Ce3+ in LuP04, transitions to four out of the five 5d 1 levels are observed as zero-phonon lines.The symmetry properties of the levels were obtained from the polarization dependence of the TPE signals.Measurements on Ce 3 + inYP0 4 support the given assignments.Although a crystal-field fit yields a satisfactory RMS energy deviation, an unrealistic value of the spin-orbit coupling parameter, ( 5 d1, is obtained.The • vibronic coupling appears to be smaller than for the single-photon absorption spectra, and the vibronic bands show a rich structure.There are striking differences between the energies and the relative intensities of the vibronic lines and the associated zero-phonon lines.The vibronic coupling is also found to be strongly dependent on the Ce 3 + concentration.78.50.Ec,42.65.-k
Near-UV excited-state absorption spectra obtained with a pulsed pump–probe technique were recorded in LiYF4:Pr3+ at 77 and at 8 K and revealed a detailed structure of the 4f2 1D2→4f5d and 4f2 (3P0+1I6)→4f5d optical transitions. These experimental results, together with those previously obtained at room temperature, are compared with the numerical predictions of a full calculation of the 4f5d sublevels and of the electric dipole transitions toward these sublevels from different states of the 4f2 configuration. The agreement is good, provided that the four adjustable parameters of the theory are taken as B20(5d)=7290 cm-1,B40(5d)=-14 900 cm-1,F0=60 557 cm-1, and 〈r〉fd=0.245 Å. The level structure of the 4f5d configuration of LiYF4:Pr3+ is shown to be dominated, as expected, by the crystal field coupling of the 5d electron but also, to a noticeable extent, by the spin–orbit coupling of the 4f electron and the Coulomb repulsion of both electrons. The former of these two interactions is somewhat more efficient than the latter in the low-energy part of the 4f5d configuration, i.e., in the spectral region where the largest amount of experimental data is currently available.
A theoretical analysis of the lowest zero-phonon 4f\ensuremath{\rightarrow}5d two-photon absorption cross section in CaF2{\mathrm{CaF}}_{2}CaF2​:Ce3+{\mathrm{Ce}}^{3+}Ce3+ is presented. The transition is parity allowed because of an interaction of the rare-earth ion with the odd-parity components of the crystal field. This interaction takes two forms. The static contribution serves to mix the 4f and 5d orbitals, while a dynamic term couples the rare-earth orbitals to the nearby ligand states. A comparison of the predicted polarization anisotropy to the experimentally measured value allows an estimate of the relative strengths of the static and dynamic terms. The theoretical estimates of both the polarization anisotropy and the absolute magnitude of the cross section compare well with the experimental results.
Recent observations of two-photon absorption within the configuration 4f 7 of Gd 3+ in LaF 3 have indicated an anomalously high line strength for the transition 8 S 7/2 to 6 P 7/2 compared with 8 S 7/2 to 6 P 5/2 and 8 S 7/2 to 6 P 3/2 . It is shown that the standard expression for the two-photon intensity is unusually small for all three transitions and that a higher-order correction, involving matrix elements of the spin-orbit interaction within the intermediate configuration 4f 6 5d, predominates. The principal term is scalar, implying (in the absence of J mixing by the crystal field) isotropic contributions to the various components of the Delta J=0 transition. The line strengths that have been observed can be accounted for reasonably well without having to invoke variations in the radial integral (4f mod r mod 5d) or inadequacies in the closure approximation. Expressions for the transition matrix elements are given for the general configuration l N .
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