Two-photon transitions of Gd3+in cubic Cs2NaGdCl6

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Abstract
Two-photon absorption spectroscopy is used to investigate the 8S7/2 → 6PJ, 6I7/2 transitions of Gd3+ ions in the cubic elpasolite Cs2NaGdCl6. The Gd3+ ions occupy a centro-symmetric site (Oh); 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 6I7/2 and 6P3/2 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 6P5/2 and 6P7/2 levels is confirmed. The occurrence of the one-photon transition to 6P3/2 is tentatively explained by the J mixing involving the 6P7/2 excited state. A qualitative analysis of the relative intensities of the transitions to the 6PJ and 6I7/2 levels is presented.