Low-Lying Energy Levels and Magnetic Susceptibility of Thulium in the Garnets

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Abstract
Susceptibility measurements on TmGaG, when analyzed in terms of a cubic crystal-field model, predict that there should be no excited energy levels lower than 104 cm−1 above the ground state. Measurement and analysis of the spectrum of thulium in three different hosts, however, reveal the presence of levels lying well below 104 cm−1 and very sensitive to the detailed surroundings of the ion. A calculation of the energy levels of Tm3+ in the known crystal field for Yb3+ in the gallium garnet shows that a low-lying Λ5 triplet is split by the noncubic field to an extent which drastically affects the susceptibility. One is led to conclude that cubic models are insufficient for prediction of macroscopic magnetic properties in ions having degenerate cubic levels very near the ground state.

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