A site population analysis of iron atoms in Fe3Si alloys with D03 superlattice structure was performed by 57Fe Mossbauer spectroscopy using crushed and annealed powder specimens with silicon concentrations of 23.3 and 25.5 at%. The Mossbauer spectra obtained were found to be superpositions of at least three six-line components. The relative intensity for each component has been analyzed using the thin foil approximation. The atomic configuration and the relative number of iron atoms of the component were determined from the values of the hyperfine field and the relative intensity for each component, and from these data the short-range-order parameter was determined.In order to determine the long-range-order parameters of the alloys, a two step procedure was used: First, the perfectly ordered D03 lattice of 25 at% Si was constructed by computer, and then atoms were replaced randomly so that any desired values of the alloy concentration and the degree of order are reached. By comparing the computer simulation with the result of the Mossbauer experiment, the long-rangeorder parameters, S(D03) and S(B2), were determined. The values agree well with those obtained by the powder X-ray diffraction technique. (Received June 12, 1985) Keywords: Mossbauer spectroscopy, site population, atomic configuration, hyperfine field order-disorder transformation, iron-silicon alloys, DO3 lattice, B2 lattice, long-range-order Parameter. short-range-order parameterAs shown in the equilibrium phase diagram, the Fe-Si alloy near room temperature has a disordered structure (bcc) when the silicon concentration is less than 10 at%, the B2 structure for 10-20 at% Si and the D03 structure for 12-25 at% Si. Especially in the composition region of 12-24 at% Si, the temperature change induces a phase transformation among D03, B2 and bccc(1).57Fe Mossbauer spectra of ferromagnetic materials show the nuclear Zeeman splitting which is caused by the hyperfine field at the nucleus. In many ferromagnetic iron alloys, the electronic state of 57Fe and the hyperfine field at 57Fe nucleus mainly depend on the surrounding atomic configuration; this is the so called local environment effect. Fe3Si and Fe3Al are typical examples of compounds which show a large local environment effect. Many 57Fe Mossbauer spectroscopic studies (besides a great number of results obtained by other methods) have been reported on these alloy systems to investigate the site populations in ordered and disordered states of these alloy systems(2)- (15) .Information which can be obtained directly from Mossbauer spectra in this alloy system depends mainly on the short-range atomic configurations. However, if it is possible to determine long-range-order parameters by Mossbauer spectra, this method is very useful to gain information on order-disorder transformations which is usually obtained from other methods such as X-ray diffraction, because data on short-range and on long-range order can be obtained at the same time. In this method, neither single crystals nor very fine powders ...