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International Conference on Luminescence - 1984

Two-Photon Excitations of Higher 5d States in Ce3+:CaF2

Swapan Kumar Gayen, Gerald J. Pogatshnik, D. S. Hamilton

Published Jan 1, 1984• 2 citations
Publisher

Abstract

The 4f-->5d near-ultraviolet transitions in Ce3+:CaF2 are dipole allowed in one-photon absorption (OPA) and first-order parity-forbidden for two-photon absorption (TPA). A relaxation of the parity selection rule due to odd crystal-field components has previously been observed1 in the TPA from the 4f ground state to the lowest 5d state. In this paper the TPA measurements are extended to include transitions to the higher 5d states.

DOI
10.1364/icol.1984.tud21

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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 density matrix resonant two-photon absorption (TPA) theory applicable to laser crystals doped with rare earth ions is described. Using this theory, resonant TPA cross sections for transitions from the ground state to the second excited state of the 4f5d configuration in Pr3+:Y3Al5O12 are calculated. The peak value of TPA cross section calculated is 2.75 × 10-50 cm4 s which is very close to the previous experimental value 4 × 10-50 cm4 s. The good agreement of calculated data with measured values demonstrates that the density matrix resonant TPA theory can predict resonant TPA intensity much better than the standard second-order perturbation TPA theory.

Journal of Physics Condensed Matter•Oct 5, 1999•0 citations
The 4f-->5d near-ultraviolet transitions in Ce3+:CaF2 are dipole allowed in one-photon absorption (OPA) and first-order parity-forbidden for two-photon absorption (TPA). A relaxation of the parity selection rule due to odd crystal-field components has previously been observed1 in the TPA from the 4f ground state to the lowest 5d state. In this paper the TPA measurements are extended to include transitions to the higher 5d states.
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.
A theoretical estimate of the two-photon absorption (TPA) cross section for the lowest 4f\ensuremath{\rightarrow}5d zero-phonon transition in Ce3+{\mathrm{Ce}}^{3+}Ce3+:CaF2{\mathrm{CaF}}_{2}CaF2​ is presented. A point-charge crystal-field model is used to calculate the odd component of the C4v{C}_{4v}C4v​ crystal field which mixes states of opposite parity into the initial and final states participating in the transition. The sum over intermediate states is evaluated by assuming a constant energy denominator and using a closure approximation. The calculated magnitude and polarization anisotropy of the TPA cross section are compared with the experimentally measured values and methods to improve the calculation are discussed.
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
Abstract The technique of two‐photon‐absorption spectroscopy with polarized laser‐light is applied to localized excitations of 4f‐electrons in crystals. The relevant selection rules are discussed. A method is outlined for the unique determination of the relative magnitude of partial transition‐probabilities with different types of symmetry using linear and circular polarization of the incident light. The anisotropy of the two‐photon absorption has been measured in single crystals of cubic CaF2:Eu2+ at five different wavenumbers. The relative intensities of transitions belonging to the three different types of symmetry active in two‐photon absorption are constant in the range of the e‐band (26,000 to 29,000 cm−1) but differ from these values at 37,700 cm−1 in the range between the e‐ and the t‐band. This result is discussed in the frame of existing interpretations of the 4f65d‐configuration of Eu2+ in CaF2.
The density matrix resonant two-photon absorption (TPA) theory applicable to laser crystals doped with rare earth ions is described. Using this theory, resonant TPA cross sections for transitions from the ground state to the second excited state of the 4f5d configuration in Pr3+:Y3Al5O12 are calculated. The peak value of TPA cross section calculated is 2.75 × 10-50 cm4 s which is very close to the previous experimental value 4 × 10-50 cm4 s. The good agreement of calculated data with measured values demonstrates that the density matrix resonant TPA theory can predict resonant TPA intensity much better than the standard second-order perturbation TPA theory.