Abstract
Measurements of the nuclear magnetic resonance of the F19 nucleus in single crystals of NiF2 have been made at temperatures between 4.2°K and 298°K. In the paramagnetic state at 298°K, for arbitrary directions of H0 two resonances were observed, while for H0 in a (100) plane only one resonance was observed as expected from the crystal symmetry. The shift of the resonances from the normal resonance field ωγN allows one to calculate three independent parameters of the hyperfine interaction between the F19 nuclei and the magnetic electrons. In conjunction with measurements made in the antiferromagnetic state, it was possible to determine the individual components of the hyperfine interaction in units of 104 cm1 as AsI=36.4±1.8, AsII=42.1±2.1, AσI=9.1±0.9, and AσII=9.9±0.9. Superscripts refer to the two different bonds with Ni++ and subscripts s and σ refer to isotropic and anisotropic contributions. From these we calculate that the fractions of unpaired spin in the corresponding fluoride ion s and pσ orbitals are fsI=(0.46±0.02)%, fsII=(0.54±0.03)%, fσI=(4.1±0.4)%, and fσII=(4.5±0.4)%. Since geometrical considerations almost completely forbid magnetic pπ interactions in NiF2, there is a negligible cancellation of pσ interactions by the