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Journal of the Optical Society of America B

Experimental and theoretical investigations of the 4ƒ^2→ 4ƒ5d ground-state and excited-state absorption spectra of Pr^3+ in LiYF_4

Mathieu Laroche, J.L. Doualan, Sylvain Girard, Jean Margerie, R. Moncorgé

Published Jul 1, 2000• 52 citations
Publisher

Abstract

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.

DOI
10.1364/josab.17.001291

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Direct calculation of correlated absorption amplitudes for Nd:LiYF4

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The correlation contribution to the transition amplitudes are investigated in the case of ${\mathrm{N}\mathrm{d}:\mathrm{L}\mathrm{i}\mathrm{Y}\mathrm{F}}_{4}.$ By using many-body perturbation theory, we derive expressions for an effective dipole operator. The operators considered are ${\ensuremath{\Omega}}_{\mathrm{es}}^{(1)\ifmmode\dagger\else\textdagger\fi{}}D{\ensuremath{\Omega}}_{\mathrm{cf}}^{(1)},$ ${\ensuremath{\Omega}}_{\mathrm{cf}}^{(1)\ifmmode\dagger\else\textdagger\fi{}}D{\ensuremath{\Omega}}_{\mathrm{es}}^{(1)},$ ${\ensuremath{\Omega}}_{\mathrm{es}\ensuremath{-}\mathrm{cf}}^{(2)\ifmmode\dagger\else\textdagger\fi{}}D,$ and $D{\ensuremath{\Omega}}_{\mathrm{es}\ensuremath{-}\mathrm{cf}}^{(2)}.$ In contrast to third-order spin-orbit and crystal-field modified amplitudes, inclusion of correlation modifies the standard second-order amplitudes significantly. A model cluster is optimized to experimental energy levels. This approach is then used to compute consistent odd and even crystal-field parameters needed for theoretical absorption spectra. As expected, it is observed that transitions occurring at small wavelengths are quite heavily influenced by correlation. The overall agreement between experimental and theoretical spectra below 600 nm (above $17000{\mathrm{cm}}^{\ensuremath{-}1})$ is greatly improved when correlation is taken into account.

Physical review. B, Condensed matter•Nov 6, 2003•6 citations
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.
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 influence of an external magnetic field on the hyperfine structure of the 3 H4(0) and 1D2(0) crystal field states of Pr3+ in LiYF4 is studied in order to find an efficient three-level Λ system. Using an experimentally determined spin Hamiltonian, we show that three-level Λ systems can be obtained with equal strengths for the optically excited transitions under various magnetic field magnitudes and orientations. An analytical analysis based on two levels is proposed to find useful magnetic fields without extensive numerical calculations and to understand the general behaviour of the system. Pr3+ hyperfine structure has also been directly calculated using a complete Hamiltonian including free ion, crystal field and magnetic interactions. A good agreement with the spin Hamiltonian approach is found for the ground state whereas the excited state results poorly reproduce the experiment. This is attributed to the low accuracy of 1D2 crystal field wavefunctions. This suggests that transition strengths ratios could be calculated directly from the crystal field Hamiltonian with improved crystal field parameters.
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 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.
The correlation contribution to the transition amplitudes are investigated in the case of Nd:LiYF4.{\mathrm{N}\mathrm{d}:\mathrm{L}\mathrm{i}\mathrm{Y}\mathrm{F}}_{4}.Nd:LiYF4​. By using many-body perturbation theory, we derive expressions for an effective dipole operator. The operators considered are ${\ensuremath{\Omega}}_{\mathrm{es}}^{(1)\ifmmode\dagger\else\textdagger\fi{}}D{\ensuremath{\Omega}}_{\mathrm{cf}}^{(1)},$ ${\ensuremath{\Omega}}_{\mathrm{cf}}^{(1)\ifmmode\dagger\else\textdagger\fi{}}D{\ensuremath{\Omega}}_{\mathrm{es}}^{(1)},$ ${\ensuremath{\Omega}}_{\mathrm{es}\ensuremath{-}\mathrm{cf}}^{(2)\ifmmode\dagger\else\textdagger\fi{}}D,$ and $D{\ensuremath{\Omega}}_{\mathrm{es}\ensuremath{-}\mathrm{cf}}^{(2)}.$ In contrast to third-order spin-orbit and crystal-field modified amplitudes, inclusion of correlation modifies the standard second-order amplitudes significantly. A model cluster is optimized to experimental energy levels. This approach is then used to compute consistent odd and even crystal-field parameters needed for theoretical absorption spectra. As expected, it is observed that transitions occurring at small wavelengths are quite heavily influenced by correlation. The overall agreement between experimental and theoretical spectra below 600 nm (above $17000{\mathrm{cm}}^{\ensuremath{-}1})$ is greatly improved when correlation is taken into account.