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Physical review. B, Condensed matter

F07 →5 DJ two-photon-absorption transitions of Sm2+ in SrF2

J.C. Gâcon, Gary W. Burdick, B. Moine, Hans Bill

Published May 1, 1993• 10 citations
Publisher

Abstract

One-color two-photon excitation spectra of the $^{7}$${\mathit{F}}_{0}$${\ensuremath{\rightarrow}}^{5}$${\mathit{D}}_{0}$ and $^{7}$${\mathit{F}}_{0}$${\ensuremath{\rightarrow}}^{5}$${\mathit{D}}_{2}$ transitions of ${\mathrm{Sm}}^{2+}$ in ${\mathrm{SrF}}_{2}$ 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}$${\mathit{F}}_{0}$${\ensuremath{\rightarrow}}^{5}$${\mathit{D}}_{0}$(${\mathit{A}}_{1\mathit{g}}$), $^{7}$${\mathit{F}}_{0}$${\ensuremath{\rightarrow}}^{5}$${\mathit{D}}_{2}$(${\mathit{E}}_{\mathit{g}}$), and $^{7}$${\mathit{F}}_{0}$${\ensuremath{\rightarrow}}^{5}$${\mathit{D}}_{2}$(${\mathit{T}}_{2\mathit{g}}$) Stark components observed at 15 K, respectively. The $^{7}$${\mathit{F}}_{0}$${\ensuremath{\rightarrow}}^{5}$${\mathit{D}}_{0}$(${\mathit{A}}_{1\mathit{g}}$) transition is observed to be isotropic within experimental error, while the ${\mathit{E}}_{\mathit{g}}$ and ${\mathit{T}}_{2\mathit{g}}$ components of the $^{7}$${\mathit{F}}_{0}$${\ensuremath{\rightarrow}}^{5}$${\mathit{D}}_{2}$ transition exhibit the anisotropic patterns expected in ${\mathrm{O}}_{\mathit{h}}$ symmetry. Calculations of two-photon transition intensities are conducted within the framework of the phenomenological model previously used for ${\mathrm{Sm}}^{2+}$ in MClF (M=Ba,Sr) and ${\mathrm{Eu}}^{3+}$ in ${\mathrm{LuPO}}_{4}$, where the rare-earth ion occupies sites of ${\mathit{C}}_{4\mathit{v}}$ and ${\mathit{D}}_{2\mathit{d}}$ symmetries, respectively. The present results are compared and contrasted with those obtained in these previous cases.

DOI
10.1103/physrevb.47.11712

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The two-photon transitions between the Stark levels of the 7F0^{7}\mathrm{F}_{0}7F0​ and 5D2^{5}\mathrm{D}_{2}5D2​ multiplets of the Sm2+{\mathrm{Sm}}^{2+}Sm2+ ion in BaClF are investigated both from an experimental and theoretical viewpoint. Direct two-photon excitation spectra of the 5D2^{5}\mathrm{D}_{2}5D2​ fluorescence resulting from an optical excitation with an infrared laser beam are presented and the polarization dependence of the observed transitions is analyzed. These new data are interpreted along the lines of a simple model which originates in the second-order theory developed by Axe [Phys. Rev. 136, A42 (1964)] for two-photon processes in complex atoms. The extension of this theory to the case of rare-earth ions embedded in crystalline fields is carried out by use of symmetry-adaptation techniques based on the use of an SU(2)\ensuremath{\supset}G∗{\mathrm{G}}^{\mathrm{*}}G∗ chain of groups. It is shown that the resulting model (limited up to second-order terms) describes correctly the relative intensities of the two-photon transitions between the Stark levels of the 7F0^{7}\mathrm{F}_{0}7F0​ and 5D2^{5}\mathrm{D}_{2}5D2​ multiplets of Sm2+{\mathrm{Sm}}^{2+}Sm2+ in BaClF.
The two-photon transition intensity of the ${(}^{7}{F}_{0}){\ensuremath{\Gamma}}_{1g}\ensuremath{\rightarrow}{\ensuremath{\Gamma}}_{1g}{(}^{5}{D}_{0})$ 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.
A crystal of SrF2{\mathrm{F}}_{2}F2​: Sm2+{\mathrm{Sm}}^{2+}Sm2+ was operated as a pulsed optical maser at temperatures close to 4.2\ifmmode^\circ\else\textdegree\fi{}K. The 6969 \AA{} output corresponds to the wavelength of an exceedingly sharp line ($\ensuremath{\Delta}\ensuremath{\nu}<0.6$ ${\mathrm{cm}}^{\ensuremath{-}1}$) in which almost all of the low-temperature fluorescence is concentrated. In contrast to what prevails in CaF2{\mathrm{F}}_{2}F2​: Sm+2{\mathrm{Sm}}^{+2}Sm+2 masers, the output is characterized by strong relaxation oscillations. This may be explained by the large difference in the fluorescent lifetimes in the two systems. While in CaF2{\mathrm{F}}_{2}F2​: Sm2+{\mathrm{Sm}}^{2+}Sm2+ the value of $\ensuremath{\tau}$ is approximately 1.5\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}6}$ sec, in SrF2{\mathrm{F}}_{2}F2​: Sm2+{\mathrm{Sm}}^{2+}Sm2+ it has a value of 15 msec. The reason for the large difference in $\ensuremath{\tau}$ values, in turn, depends upon the relative proximity of the long-wavelength edge of the red band to the position of the metastable 5D0^{5}D_{0}5D0​ level from which fluorescence occurs. Absorption measurements taken at helium temperatures on SrF2{\mathrm{F}}_{2}F2​: Sm2+{\mathrm{Sm}}^{2+}Sm2+ show that the lowest vibrational level of the lowest lying $4f\ensuremath{-}5d$ band lies \ensuremath{\sim}600 ${\mathrm{cm}}^{\ensuremath{-}1}$ above the position of the 5D0^{5}D_{0}5D0​ level while in CaF2{\mathrm{F}}_{2}F2​: Sm2+{\mathrm{Sm}}^{2+}Sm2+ there is near coincidence of the corresponding levels and consequently strong configurational mixing. Crystals of SrCl2{\mathrm{Cl}}_{2}Cl2​: Sm2+{\mathrm{Sm}}^{2+}Sm2+ were also studied in this regard and display an expected close similarity in spectral characteristics to SrF2{\mathrm{F}}_{2}F2​: Sm2+{\mathrm{Sm}}^{2+}Sm2+. The vibrational structure on the $4f\ensuremath{-}5d$ bands is much more pronounced, however, than in CaF2{\mathrm{F}}_{2}F2​: Sm2+{\mathrm{Sm}}^{2+}Sm2+ and SrF2{\mathrm{F}}_{2}F2​: Sm2+{\mathrm{Sm}}^{2+}Sm2+, indicating weaker coupling to the lattice in the excited 5d5d5d state. A tentative interpretation for the splitting of the red band seen in the absorption spectra of Sm2+{\mathrm{Sm}}^{2+}Sm2+ ions is given.
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