The magnetic structure factors of MnAlGe (space groupP4/nmm) measured with polarised neutrons have been expressed in terms of the magnetic moment of the Mn atom (site symmetry tetrahedral with tetragonal distortion), the Bessel transforms 〈j_n〉 of the Mn radial functions and the fractional occupancies of the moment density in the various crystal field orbitals. The measured structure factors were least-squares fitted with the theoretical expression involving 〈j_n〉 appropriate to the Mn⁰, Mn⁺ and Mn²⁺ atoms. The best fit was got using Mn⁰ transforms, yielding 1·45µ_B as the Mn magnetic moment. The fractional occupancies of the moment density in the crystal field orbitalsA_1g,B_1gE_g andB_2g were obtained. This analysis shows the magnetic moment to be highly non-spherical with a large fractional occupancy (38%) in theA_1g orbital directed along the tetragonal axis while the fractional occupancies ofB_1g andB_2g are found to be 31% and 30% respectively. The fractional occupancy of the moment in theE_g orbital directed towards the Ge and Al atoms is very low (1%). The spatially averaged moment density of Mn in MnAlGe is more diffuse than that of Mn I and Mn II in isostructural Mn₂Sb.

A polarised neutron study of the ferromagnetic Heusler alloy Cu₂Mn_0.863Al_1.057 has been made. It has been concluded that the magnetic moment density is primarily situated on the Mn ions. On assigning the Mn-moment value, the observed magnetic form factor is found to be in good agreement with the Mn²⁺ free ion form factor calculated by Watson and Freeman. A slight asphericity has been observed in the moment density. It is estimated that there are about 3% excess 3d-electrons in the Eg states compared to spherical distribution. There is evidence of a very small positive polarisation of the Cu atoms. No appreciable conduction electron polarisation is found.

Using polarised neutrons, the full three-dimensional magnetic structure amplitudes in the Ni_1−c Ru_c single crystals forc = 0·027, 0·033 and 0·046 were measured. Moment density maps in various portions of the Wigner-Seitz cell were obtained. It is seen from these maps that unlike Ni-based alloys with 3d impurities, the introduction of Ru to the Ni matrix produces extensive perturbations in the diffuse moment density, giving rise to a netpositive diffuse moment which tends to increase with Ru concentration. The asphericity of the host moment at first increases and then decreases with increasing Ru content. Another significant outcome of the present study is the evidence for the reversal of the sign of the Ru moment, from negative to positive, obtained by comparing the shape of the spherical site form factors of the three-alloy concentrations with the Ni spherical form factor itself. The sign reversal of the impurity moment is confirmed by the form factor analyses. Strong local environmental effects seem to play a major role in this alloy system.

The basic principle for the production of polarised thermal neutrons is discussed and the choice of various crystal monochromators surveyed. Brief mention of broad-spectrum polarisers is made. The application of polarised neutrons to the study of magnetisation density distributions in magnetic crystals, the dynamic concept of polarisation, principle and use of polarisation analysis, the neutron spin-echo technique are discussed.

The magnetic structures of Fe₄N and Mn₄N have been redetermined using neutron diffraction. The magnetic form factors, obtained from polarised neutron data have been shown to be different for the face-centred and corner atoms. A qualitative explanation of the structures of Fe₄N and Mn₄N has been provided from the shapes of the magnetic form factors.