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Physical review. B, Condensed matter

Analysis of (7F0)Γ1g→Γ1g(5D0) two-photon transition of Sm2+ in SrF2

Mason Chua, Peter A. Tanner

Published Oct 1, 1997• 3 citations
Publisher

Abstract

The two-photon transition intensity of the ${(}^{7}{F}_{0}){\ensuremath{\Gamma}}_{1g}\ensuremath{\rightarrow}{\ensuremath{\Gamma}}_{1g}{(}^{5}{D}_{0})$ transition of the ${4f}^{6}$-ion ${\mathrm{Sm}}^{2+}$ in ${\mathrm{SrF}}_{2}$ has been investigated both in Judd-Pooler and direct formalisms. Although the agreement between the different calculations may be regarded as satisfactory, the direct calculation provides additional information concerning the transition intensity mechanism. The dominant pathway is found to involve the ${4f}^{5}{5d}^{1}$ intermediate core state ${}^{6}H.$ The effects of changing the intermediate state baricenter have been investigated for both calculations, and the Judd-Pooler calculation becomes closer in agreement with the direct calculation as the energy baricenter increases.

DOI
10.1103/physrevb.56.7967

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The two-photon transition intensity of the (7F0)\ensuremathΓ1g\ensuremath→\ensuremathΓ1g(5D0){(}^{7}{F}_{0}){\ensuremath{\Gamma}}_{1g}\ensuremath{\rightarrow}{\ensuremath{\Gamma}}_{1g}{(}^{5}{D}_{0})(7F0​)\ensuremathΓ1g​\ensuremath→\ensuremathΓ1g​(5D0​) transition of the 4f6{4f}^{6}4f6-ion Sm2+{\mathrm{Sm}}^{2+}Sm2+ in SrF2{\mathrm{SrF}}_{2}SrF2​ has been investigated both in Judd-Pooler and direct formalisms. Although the agreement between the different calculations may be regarded as satisfactory, the direct calculation provides additional information concerning the transition intensity mechanism. The dominant pathway is found to involve the 4f55d1{4f}^{5}{5d}^{1}4f55d1 intermediate core state 6H.{}^{6}H.6H. The effects of changing the intermediate state baricenter have been investigated for both calculations, and the Judd-Pooler calculation becomes closer in agreement with the direct calculation as the energy baricenter increases.
One-color two-photon excitation spectra of the 7^{7}7F0{\mathit{F}}_{0}F0​${\ensuremath{\rightarrow}}^{5}$D0{\mathit{D}}_{0}D0​ and 7^{7}7F0{\mathit{F}}_{0}F0​${\ensuremath{\rightarrow}}^{5}$D2{\mathit{D}}_{2}D2​ transitions of Sm2+{\mathrm{Sm}}^{2+}Sm2+ in SrF2{\mathrm{SrF}}_{2}SrF2​ have been measured at low temperature and their dependences upon photon polarization analyzed. Linewidths on the order of 0.2, 0.6, and 1.0 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ are obtained for the 7^{7}7F0{\mathit{F}}_{0}F0​${\ensuremath{\rightarrow}}^{5}$D0{\mathit{D}}_{0}D0​(A1g{\mathit{A}}_{1\mathit{g}}A1g​), 7^{7}7F0{\mathit{F}}_{0}F0​${\ensuremath{\rightarrow}}^{5}$D2{\mathit{D}}_{2}D2​(Eg{\mathit{E}}_{\mathit{g}}Eg​), and 7^{7}7F0{\mathit{F}}_{0}F0​${\ensuremath{\rightarrow}}^{5}$D2{\mathit{D}}_{2}D2​(T2g{\mathit{T}}_{2\mathit{g}}T2g​) Stark components observed at 15 K, respectively. The 7^{7}7F0{\mathit{F}}_{0}F0​${\ensuremath{\rightarrow}}^{5}$D0{\mathit{D}}_{0}D0​(A1g{\mathit{A}}_{1\mathit{g}}A1g​) transition is observed to be isotropic within experimental error, while the Eg{\mathit{E}}_{\mathit{g}}Eg​ and T2g{\mathit{T}}_{2\mathit{g}}T2g​ components of the 7^{7}7F0{\mathit{F}}_{0}F0​${\ensuremath{\rightarrow}}^{5}$D2{\mathit{D}}_{2}D2​ transition exhibit the anisotropic patterns expected in Oh{\mathrm{O}}_{\mathit{h}}Oh​ symmetry. Calculations of two-photon transition intensities are conducted within the framework of the phenomenological model previously used for Sm2+{\mathrm{Sm}}^{2+}Sm2+ in MClF (M=Ba,Sr) and Eu3+{\mathrm{Eu}}^{3+}Eu3+ in LuPO4{\mathrm{LuPO}}_{4}LuPO4​, where the rare-earth ion occupies sites of C4v{\mathit{C}}_{4\mathit{v}}C4v​ and D2d{\mathit{D}}_{2\mathit{d}}D2d​ symmetries, respectively. The present results are compared and contrasted with those obtained in these previous cases.
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Eighteen selected two-photon absorption (TPA) transition line strengths with polarization angles θ = 0° and 45°, spanning several orders of magnitude, have been calculated for the Tb 3+ ion in the cubic host Cs 2 NaTbCl 6 . The results are in reasonable agreement with experimental results in the literature. The calculation utilized the crystal field (CF) wavefunctions for the initial and final states of the 4f 8 configuration, and utilized free ion or CF wavefunctions (with the corresponding energies) for 4f 7 core states of the whole intermediate 4f 7 5d configuration comprising 34 320 states. The intensities of certain transitions were found to be very sensitive to the inclusion of the CF interaction within the 4f 7 core. In contrast to previous fourth- or third-order calculations of the TPA transition line strength of the strong transition ( 7 F 6 )A 1g → ( 5 D 4 )A 1g using pure Russell–Saunders (RS) wavefunctions for the | 7 F 6 ⟩ initial and ⟨ 5 D 4 | final states, our second-order direct calculation shows that the admixed RS wavefunctions |[ 7 F 6 ]⟩ and ⟨[ 5 D 4 ]| must be used to account for its high intensity. The effects of CF interactions within the 4f 7 core, i.e. J -mixing and CF energy level splitting, upon the ( 7 F 6 )A 1g → ( 5 D 4 )E g TPA transition line strength have been separated, and the latter effect is shown to be more important for the transition investigated.
The $4{f}^{6}\phantom{\rule{0.28em}{0ex}}{}^{7}{F}_{0}\ensuremath{\rightarrow}4{f}^{6}{}^{5}{D}_{0}$ intraconfiguration transition in Sm:SrF2\mathrm{Sm}:{\mathrm{SrF}}_{2}Sm:SrF2​ is forbidden for Sm2+{\mathrm{Sm}}^{2+}Sm2+ ions in the octahedrally symmetric substitution sites in SrF2{\mathrm{SrF}}_{2}SrF2​. We report the direct observation of this transition using laser-induced fluorescence at cryogenic temperatures, and measurements of the excited-state lifetime and the excitation cross section. To the best of our knowledge, this optical transition has the longest-lived excited state ever observed in a solid.