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physica status solidi (b)

Two‐Photon Excitation Spectra of Trivalent Rare‐Earth Ion Luminescence in Crystals

Pavel A Apanasevich, R. I. Gintoft, V. S. Korol'kov, A. G. Makhanek, G. A. Skripko

Published Aug 1, 1973• 41 citations
Publisher

Abstract

Abstract Theoretical and experimental investigations are made of two‐photon absorption spectra of trivalent rare‐earth ions in crystals. Effective cross‐sections, selection rules, and relative intensities of the components are found. The most intensive two‐photon transitions are established. Two‐photon excitation spectra of luminescence of Er3+ and Ho3+ ions in CaF2 are obtained and effective excitation cross‐sections are measured using a tunable dye laser (715 to 850 nm). It is shown that the spectra have a peculiar structure which differs considerably from that of the one‐photon absorption spectra. The experimental results agree with theory. It is established that one of the levels in Ho3+ is the level 5G6 rather than 3K7 usually assumed.

DOI
10.1002/pssb.2220580236

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Two‐Photon Absorption of CaF2:Eu2+

Eberhard G. Bayer, Gerhard Schaack

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.

physica status solidi (b)•Jan 1, 1970•37 citations
Abstract Theoretical and experimental investigations are made of two‐photon absorption spectra of trivalent rare‐earth ions in crystals. Effective cross‐sections, selection rules, and relative intensities of the components are found. The most intensive two‐photon transitions are established. Two‐photon excitation spectra of luminescence of Er3+ and Ho3+ ions in CaF2 are obtained and effective excitation cross‐sections are measured using a tunable dye laser (715 to 850 nm). It is shown that the spectra have a peculiar structure which differs considerably from that of the one‐photon absorption spectra. The experimental results agree with theory. It is established that one of the levels in Ho3+ is the level 5G6 rather than 3K7 usually assumed.
To study the role of stepwise and relaxation processes under effective excitation of anti-Stokes luminescence of rare-earth (RE) ions in crystals the time-shifted pulse method is used. It is shown that direct comparison of measured single- and two-photon luminescence excitation spectra often enables one to make immediate conclusions on the position and classification of electron levels of RE ions. The Tb3+ and Eu3− level structures (crystal CaF2) in the near ultraviolet are considered as an example. The peculiarities connected with the polarization characteristics of the two-photon absorption of radiation by the trivalent RE ions in a crystal matrix are discussed. To obtain the two-photon spectra a frequency-tunable organic dye solution laser (ODSL) is used.
The polarised two-photon (IR) and one-photon (visible) luminescence excitation spectra of Nd 3+ nanoclusters in CaF 2 and SrF 2 crystals are measured at 10 K using a :LiF colour centre laser tunable in spectral ranges 1090 — 1230 nm and 545 — 615 nm with an emission linewidth of ~0.02 — 0.03 cm -1 , an average output power of ~55 mW, and a pulse repetition rate of 10 Hz. The two-photon excitation spectra at the 4 I 9/2 → 4 G 5/2 transition reveal the structure, which is absent upon one-photon excitation, which can be explained by different selection rules for some Stark — Stark transitions upon one- and two-photon absorption.
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.
The observation of two-photon absorption by a very efficient up-converted emission is reported for Ho3+{\mathrm{Ho}}^{3+}Ho3+ in CaF2{\mathrm{F}}_{2}F2​, SrF2{\mathrm{F}}_{2}F2​, and CdF2{\mathrm{F}}_{2}F2​ 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 AAA is excited by the dye-laser photons of frequencies 15 400-15 700 ${\mathrm{cm}}^{\ensuremath{-}1}$: The band BBB is excited by the dye-laser photons of frequencies 15 800-16 400 ${\mathrm{cm}}^{\ensuremath{-}1}$. No one-photon absorption is observed for Ho3+{\mathrm{Ho}}^{3+}Ho3+ 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 AAA and BBB arise from two different modes of two-photon excitation. The band AAA 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 BBB 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.
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.