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Journal of Luminescence

Direct two-photon absorption of Gd(OH)3 and GdCl3 in an applied magnetic field

B. Jacquier, Y. Salem, C. Linarès, J.C. Gâcon, Rachid Mahiou, R. L. Cone

Published Dec 1, 1987• 14 citations
Publisher
DOI
10.1016/0022-2313(87)90121-9

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AIP conference proceedings•Jan 1, 1973•1 citation
The authors report a detailed analysis of the intensity and polarisation dependence of the 8 S 7/2 to 6 P 7/2 two-photon transition Stark components of Gd 3+ in the concentrated magnetic insulator Gd(OH) 3 under an applied magnetic field (up to 3.5 T) at very low temperature (2 K). The experimental technique consisted of detecting the ultraviolet 6 P 7/2 to 8 S 7/2 one-photon fluorescent emission resulting from two-photon excitation in the 6 P 7/2 states, using a single pulsed dye-laser beam. The standard second-order theory of Axe is shown to fail in explaining the relative intensities of the Stark components. This is especially true in the case of the Delta M=0 transitions for which strong disagreements are observed. It is shown that the introduction of the third-order contribution involving the spin-orbit interaction within the 4f 6 5d states allows the experimental spectra to be reproduced in a correct way. Finally the effects of ion-ion interactions on the two-photon line profiles are discussed.
We report the observation of a magnon sideband in the 6P7/2 ⇐ 8S7/2 optical absorption spectrum of Gd+3 in the ferromagnetic insulator GdCl3. The transition energy and its dependence on magnetic field demonstrate this to arise from the simultaneous excitation of a magnon and optical exciton. The decrease in its intensity with increasing magnetic field suggest the source of its intensity is directly connected with the zero‐point spin deviations which occur in a ferromagnet possessing significant magnetic dipolar interactions. The magnitude of the intensity is shown to be consistent with a single‐ion transition mechanism which because of the zero‐point spin deviations allows a small probability for a double‐excitation process. This transition mechanism is distinct from that responsible for the previously observed magnon sidebands in the transition‐metal magnetic insulators.