The structure and magnetic properties of nanocrystalline PrCo3 prepared by high-energy milling technique have been investigated by means of X-ray diffraction using the Rietveld method coupled to Curie temperature and magnetic measurements. The as-milled samples were subsequently annealed in temperature range from 750 to 1050• C for 30 min to optimize the extrinsic properties. From x-ray studies of magnetic aligned samples, the magnetic anisotropy of this compounds is found uniaxial. The Curie temperature is 349 K and no saturation reached at room temperature for applied field of 90 kOe. The coercive field of 55 kOe and 12 kOe measured at 10 and 293 K respectively is obtained after annealing at 750• C for 30 min suggests that nanocrystalline PrCo3 are interesting candidates in the field of permanent magnets. We have completed this experimental study by simulations in the micromagnetic framework in order to get a qualitative picture of the microstructure effect on the macroscopic magnetization curve. From this simple model calculation, we can suggest that the after annealing the system behaves as magnetically hard crystallites embedded in a weakly magnetized amorphous matrix.

Nanocrystalline PrCo(3) powder has been synthesized by high-energy milling and was subsequently annealed from 873 to 1273 K for 30 min to optimize the extrinsic properties. The structure and magnetic properties of the nanocrystalline PrCo(3) have been investigated by means of x-ray and neutron diffraction as well as magnetization measurements. All compounds crystallize in the same PuNi(3) type structure, with grain sizes between 28 and 47 nm. As the annealing temperature increases, a maximum coercive field of 12 kOe at 300 K (55 kOe at 10 K) was obtained by annealing at 1023 K for a grain size of 35 nm. The refinement of the neutron powder diffraction patterns (NPD) of PrCo(3) from 1.8 to 300 K shows an expansion of the parameter a and a contraction of the parameter c, leading to a decrease of the ratio c/a. The evolution of the Co and Pr magnetic sublattices measured by NPD indicates that this compound is a highly anisotropic uniaxial ferromagnet with the easy magnetization axis parallel to c(-->). This experimental study has been completed by a theoretical investigation of the electronic structure of the PrCo(x) (x = 2, 3 and 5) compounds. Band structure calculations with collinear spin polarization were performed by using the local approximation of the density functional theory scheme implemented in the projector-augmented wave method. The electronic structure of PrCo(3) compound in both directions of spin shows that the majority of occupied states are dominated by the 3d states of Co, with a strong electronic charge transfer from Pr to Co. The PrCo(3) electronic structure can be explained by a superimposition of those of PrCo(2) and PrCo(5), as expected from its crystal structure. The magnetic anisotropy has been confirmed for PrCo(3), as a non-collinear spin calculation with the polarization along the c axis is shown to be more stable than with the polarization in the (a(-->),b(-->)) plane.