Magnetic Interactions between Rare-Earth Ions in Insulators. II. Electron-Paramagnetic-Resonance Measurements of Gd3+ Pair and Gd3+-Eu3+ Interaction Constants in EuCl3

Abstract
Paramagnetic resonance has been observed from both single ions and isolated pairs of Gd3+ in EuCl3 at 77°K and 25.6 GHz. The pair spectra were analyzed in the same way as those observed previously from Gd3+ in LaCl3. The results give accurate values for the interaction parameters between both nearest (nn) and next-nearest neighbors (nnn). The dominant terms are of the form of isotropic exchange (JS1·S2), with Jnn(pair)=0.0488±0.0010 cm1 and Jnnn(pair)=0.0637±0.0020 cm1. The anisotropic parts of the interactions could be accounted for completely by the calculated magnetic dipole-dipole coupling. Combining these results with earlier measurements in LaCl3, good estimates can be made of the exchange interactions in pure GdCl3: Jnn(GdCl3)=0.056±0.006 cm1 and Jnnn(GdCl3)=0.064±0.003 cm1. These values are in excellent agreement with those inferred from analyses of susceptibility and specific-heat measurements, and they resolve unambiguously earlier uncertainties in the choice of possible parameters. The magnitudes and even the signs of the interactions remain unexplained. From measured g-value shifts relative to Gd3+ in LaCl3 it was also possible to estimate the isotropic part of the Gd3+-Eu3+ exchange interaction: Jnn(GdEu)=0.052±0.030 cm1 and Jnnn(Gd