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Journal of Alloys and Compounds

4th-order contributions to the s-8(7/2)-]i-6(17/2) 2-photon transition of gd3+ in a cubic lattice

Arnout Jozef Ceulemans, G. M. Vandenberghe

Published Jan 1, 1994• 0 citations
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Two-photon absorption spectroscopy is used to investigate the 8 S 7/2 → 6 P J , 6 I 7/2 transitions of Gd 3+ ions in the cubic elpasolite Cs 2 NaGdCl 6 . The Gd 3+ ions occupy a centro-symmetric site (O h ); so the odd terms of the crystal field vanish and the pure electric dipole transitions should not be observed in one-photon experiments. As a consequence the electric dipole allowed two-photon transitions involving the 6 I 7/2 and 6 P 3/2 excited states are well observed in contrast with their weakness in the one-photon spectrum. Furthermore the magnetic dipole character of the transitions to the 6 P 5/2 and 6 P 7/2 levels is confirmed. The occurrence of the one-photon transition to 6 P 3/2 is tentatively explained by the J mixing involving the 6 P 7/2 excited state. A qualitative analysis of the relative intensities of the transitions to the 6 P J and 6 I 7/2 levels is presented.
The energy levels of Gd3+{\mathrm{Gd}}^{3+}Gd3+ in the 6P^{6}\mathrm{P}6P, 6I^{6}\mathrm{I}6I, and 6D^{6}\mathrm{D}6D 4f7{f}^{7}f7 configuration in cubic, tetragonal, and cluster sites in CaF2{\mathrm{CaF}}_{2}CaF2​ have been excited by two-photon absorption. The relative two-photon intensities and polarization dependence show behavior which is similar to that previously observed for Gd3+{\mathrm{Gd}}^{3+}Gd3+:LaF3{\mathrm{LaF}}_{3}LaF3​ and Eu2+{\mathrm{Eu}}^{2+}Eu2+:CaF2{\mathrm{CaF}}_{2}CaF2​ and which requires higher-order perturbation theory in the virtual intermediate 4${f}^{6}$5d configuration.