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Physical review. B, Condensed matter

Resonant enhancement of two-photon transitions to the second excited 4f5dstate in Pr3+ : Y3 Al5 O12

Bin Qing Xie, Y. M. Cheung, Swapan Kumar Gayen

Published Mar 1, 1993• 9 citations
Publisher

Abstract

The two-photon absorption cross section for transitions from the $^{3}$${\mathit{H}}_{4}$ ground-state manifold to the second excited state of the 4f5d configuration of ${\mathrm{Pr}}^{3+}$ in ${\mathrm{Y}}_{3}$${\mathrm{Al}}_{5}$${\mathrm{O}}_{12}$ is observed to be enhanced by about two orders of magnitude when the excitation frequency happens to be resonant with the $^{3}$${\mathit{P}}_{\mathit{J}}$ (J=0,1,2) and $^{1}$${\mathit{I}}_{6}$ intermediate states of the 4${\mathit{f}}^{2}$ configuration. The structure and line shape of the two-photon excitation spectrum spanning the 39 600--46 950 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ transition-energy range are entirely dominated by these resonantly enhanced transitions, while the contributions from nonresonant transitions appear as a slowly varying background beneath the strong resonance peaks. A two-photon absorption cross section as high as 4\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}50}$ ${\mathrm{cm}}^{4}$ s is measured at the peak of the resonantly enhanced transition at 44 246 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$, which involves a level of the $^{3}$${\mathit{P}}_{2}$ manifold as the intermediate state. The spectrally integrated cross section over that manifold is 3.3\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}38}$ ${\mathrm{cm}}^{4}$.

DOI
10.1103/physrevb.47.5557

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4f2to 4f5d excited state absorption in Pr3+:YAlO3

S Nicolas, Mathieu Laroche, S Girard +5 more

Excited-state absorption spectra, from the 3 P J - 1 I 6 or 1 D 2 manifold to 4f5d levels, recorded in the 23000 - 42000 cm -1 range and calibrated in units of cross sections, are reported and discussed in the case of Pr 3+ -doped YAlO 3 . The 4f5d 4f 2 Pr 3+ emission between 30000 and 44000 cm -1 is then observed, showing the possibility of UV laser operation following two-step excitation pumping using near-UV-visible pump photons.

Journal of Physics Condensed Matter•Sep 24, 1999•35 citations
The two-photon absorption cross section for transitions from the ^{3}$${\mathit{H}}_{4} ground-state manifold to the second excited state of the 4f5d configuration of Pr3+{\mathrm{Pr}}^{3+}Pr3+ in {\mathrm{Y}}_{3}$${\mathrm{Al}}_{5}$${\mathrm{O}}_{12} is observed to be enhanced by about two orders of magnitude when the excitation frequency happens to be resonant with the ^{3}$${\mathit{P}}_{\mathit{J}} (J=0,1,2) and ^{1}$${\mathit{I}}_{6} intermediate states of the 4f2{\mathit{f}}^{2}f2 configuration. The structure and line shape of the two-photon excitation spectrum spanning the 39 600--46 950 cm\ensuremath−1{\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}cm\ensuremath−1 transition-energy range are entirely dominated by these resonantly enhanced transitions, while the contributions from nonresonant transitions appear as a slowly varying background beneath the strong resonance peaks. A two-photon absorption cross section as high as 4\ifmmode\times\else\texttimes\fi{}10\ensuremath−50{10}^{\mathrm{\ensuremath{-}}50}10\ensuremath−50 cm4{\mathrm{cm}}^{4}cm4 s is measured at the peak of the resonantly enhanced transition at 44 246 cm\ensuremath−1{\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}cm\ensuremath−1, which involves a level of the ^{3}$${\mathit{P}}_{2} manifold as the intermediate state. The spectrally integrated cross section over that manifold is 3.3\ifmmode\times\else\texttimes\fi{}10\ensuremath−38{10}^{\mathrm{\ensuremath{-}}38}10\ensuremath−38 cm4{\mathrm{cm}}^{4}cm4.
The optical-absorption transitions originating from the lowest 4f5d excited state of Pr3+{\mathrm{Pr}}^{3+}Pr3+ in Y3{\mathrm{Y}}_{3}Y3​Al5{\mathrm{Al}}_{5}Al5​O12{\mathrm{O}}_{12}O12​ have been studied. The experimental arrangement uses a 7-ns 266-nm light pulse to populate the lowest 4f5d state, and a spatially overlapped, time-sequenced pulse from a frequency-tunable dye laser to induce transitions from that excited state. The excited-state-absorption (ESA) spectrum covering the 900--300-nm probe wavelength range is characterized by two broad peaks centered at 700 and 350 nm on a slowly rising background. The peak ESA cross section at 355 nm is (1\ifmmode\pm\else\textpm\fi{}0.1)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}17}$ cm2{\mathrm{cm}}^{2}cm2. The position, shape, and strength of the spectrum suggest that the terminal states of the ESA transitions are the second 4f5d state of Pr3+{\mathrm{Pr}}^{3+}Pr3+ and the conduction band of the host lattice. The ESA measurements have been extended to transitions from the 3^{3}3P0{\mathit{P}}_{0}P0​ and 1^{1}1D2{\mathit{D}}_{2}D2​ excited states of the 4f2{\mathit{f}}^{2}f2 configuration of Pr3+{\mathrm{Pr}}^{3+}Pr3+ as well. The ESA cross sections at a probe wavelength of 532 nm are (8\ifmmode\pm\else\textpm\fi{}1)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}19}$ cm2{\mathrm{cm}}^{2}cm2 and (5.7\ifmmode\pm\else\textpm\fi{}0.6)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}19}$ cm2{\mathrm{cm}}^{2}cm2 for transitions from the 3^{3}3P0{\mathit{P}}_{0}P0​ and 1^{1}1D2{\mathit{D}}_{2}D2​ excited states, respectively. The terminal state of ESA transitions from these two levels is the lowest 4f5d state. The strong ESA completely inhibits the potential laser action based on emission from these states in this crystal.
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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.
Resonant enhancement by a factor of over 20 of direct two-photon absorption from the ground state 7F6^{7}\mathrm{F}_{6}7F6​ to the excited state 5G6^{5}\mathrm{G}_{6}5G6​ of the 4f8{f}^{8}f8 configuration of the Tb3+{\mathrm{Tb}}^{3+}Tb3+ 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 7F6^{7}\mathrm{F}_{6}7F6​${\mathrm{\ensuremath{-}}}^{5}$D4{\mathrm{D}}_{4}D4​ resonance, a much stronger contribution arose from the 4f8{f}^{8}f8 configuration 5D4^{5}\mathrm{D}_{4}5D4​ intermediate state. Two-photon absorption was clearly isolated from two-step (incoherent) excitation by varying the timing of two separately triggered lasers.