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Journal of Physics Condensed Matter

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

S Nicolas, Mathieu Laroche, S Girard, R. Moncorgé, Yannick Guyot, M.‐F. Joubert, E Descroix, Ashot G. Petrosyan

Published Sep 24, 1999• 35 citations
Publisher

Abstract

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.

DOI
10.1088/0953-8984/11/40/317

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Acta Physica Sinica•Jan 1, 2005•2 citations
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.
Excited-state absorption spectra obtained by a pulsed pump–probe technique specially designed for the near-UV spectral domain were recorded in three Pr3+-doped fluoride crystals (KY3F10,LiYF4, and BaY2F8). These excited-state absorption spectra correspond to optical transitions from the 3P0 or the 1D2 metastable levels of the 4f2 configuration up to the first energy levels of the 4f5d electronic configuration. The position, the anisotropic behavior, and the line shape of the observed excited-state absorption bands are discussed and compared with ground-state absorption (from level 3H4) or direct excitation spectra available in the literature. Subsequently, two-step excitation into the 4f5d high-lying energy levels of Pr3 by means of 3P0 and 1D2 is shown to be an efficient way to produce broadband UV fluorescence by use of pump beams in the blue and the near UV.
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.
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.
We excite the (4f2)1s0 state directly through a two photon excited state absorption (from the 1D2 level) and indirectly through excitation of the 4f5d band (using an ArF excimer laser). In Pr3+:LaF3 the 1S0 state lies below the band, and only 1S0 emission is observed. In most hosts examined, it is above the band, and only 4f5d emission is observed. In Pr3+:CaF2 there are sites with each of these properties, and both 1S0 and 4f5d emission are observed, with a relative strength that is concentration dependent.
The two-photon absorption cross section for transitions from the 3^{3}3H4{\mathit{H}}_{4}H4​ ground-state manifold to the second excited state of the 4f5d configuration of Pr3+{\mathrm{Pr}}^{3+}Pr3+ in Y3{\mathrm{Y}}_{3}Y3​Al5{\mathrm{Al}}_{5}Al5​O12{\mathrm{O}}_{12}O12​ is observed to be enhanced by about two orders of magnitude when the excitation frequency happens to be resonant with the 3^{3}3PJ{\mathit{P}}_{\mathit{J}}PJ​ (J=0,1,2) and 1^{1}1I6{\mathit{I}}_{6}I6​ 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 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ 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{}${10}^{\mathrm{\ensuremath{-}}50}$ cm4{\mathrm{cm}}^{4}cm4 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^{3}3P2{\mathit{P}}_{2}P2​ manifold as the intermediate state. The spectrally integrated cross section over that manifold is 3.3\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}38}$ cm4{\mathrm{cm}}^{4}cm4.
Yttrium aluminum garnet (YAG): Pr3+ is synthesized by codeposition me thod. Vacuum ultraviolet (VUV) excitation and emission spectra of YAG: Pr3+ at different temperatures are measured using synchrotron radiation as an excitation source. We analyze the transition process after excitation to 4f5d en ergy band and estimate the Huang-Rhys factor S and phonon energy ηω of YAG: Pr 3+ by multi-phonon relaxation. Emission of self-trapped exciton (STE) and 3P0→3H4,5,6 emission transferr ed from the STE energy appear when YAG: Pr3+is excited by 170nm, whic h is a different transition process from those excited by 240nm and 289nm.