Abstract

The paper reports for the first time the experimental results of the measurements of magnetic susceptibilities ( K ⊥ and K |) and their anisotropy (Δ K) between 300 and 21.8 K and the optical absorption spectra (UV region) at 12.5 K on single crystals of gadolinium pyrogermanate (GdPG). The anisotropy, which is only 211×10 -6 emu/mol at room temperature and increases by two orders of magnitude at 21 K, is predominantly a crystal field (CF) effect on the 8S 7 2 ground term, through higher order perturbations. Interpretation of the observed magnetic data was carried out by considering a conventional spin Hamiltonian ( H s) to derive expressions for K ⊥ and K | in terms of four effective crystal field parameters (ECFP). The value s of ECFP were varied to obtain a very close fitting between the theoretical and experimental values of K ⊥, K |, δ K and K̄ The splitting of the 8S 7 2 term corresponding to these values of ECFP was found to be large, which suggests a strong CF effect in GdPG, as also observed in other RPG crystal studied earlier. The thermal characteristics of the magnetic anisotropy below 30 K deviate by about 5% which could not be explained by CF effects alone. A series expansion method was adopted to analyse the results of K ⊥ and K | below 30 K, however the corresponding coefficient B 2α and B 3α were observed t o be unusually high indicating the presence of CF effect even in this temperature region. The Schottky specific heat, C sch, between 300 and 21 K for GdPG has been calculated and this shows a maximum at T max=17 K.

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