Structural and magnetic properties of Fe 1 x Mn x 3 P x < 0.25 A. Broddefalk Department of Materials Science, Uppsala University, Box 534 SE-715 21, Uppsala, Sweden P. James Department of Physics, Uppsala University, Box 530 SE-751 21, Uppsala, Sweden Hui-Ping Liu Department of Inorganic Chemistry, Uppsala University, Box 538 SE-751, Uppsala, Sweden B. Kalska Department of Physics, Uppsala University, Box 530 SE-751 21, Uppsala, Sweden and The Soltan Institute for Nuclear Studies, 05-400 Otwock-Swierk, Poland Y. Andersson Department of Inorganic Chemistry, Uppsala University, Box 538 SE-751, Uppsala, Sweden P. Granberg and P. Nordblad Department of Materials Science, Uppsala University, Box 534 SE-715 21, Uppsala, Sweden L. Ha ¨ ggstro ¨ m and O. Eriksson Department of Physics, Uppsala University, Box 530 SE-751 21, Uppsala, Sweden Received 10 June 1999 Structural and magnetic properties of (Fe 1-x Mn x ) 3 P compounds have been investigated by means of x-ray and neutron diffraction experiments, magnetization measurements, Mo ¨ssbauer experiments, and first principles calculations. The Curie temperature of the system decreases linearly and rapidly with increasing Mn content. The zero temperature saturation magnetization, the local magnetic moments, as well as the hyperfine fields on the different metal positions of the system all decrease with increasing Mn content. The theoretical calcula- tions, on the other hand, predict an increasing magnetic moment on the metal positions with increasing Mn content. This apparent discrepancy is discussed in the light of a good agreement between experimental and theoretical results for the Co-substituted sister compounds (Fe 1-x Co x ) 3 P. I. INTRODUCTION The magnetic properties of Fe 3 P and substitutions of 3d elements for the Fe atoms are of considerable interest. 1–7 Fe 3 P is a ferromagnetic compound with a Curie temperature of 692 K Ref. 5and a saturation magnetization of 1.70 B /Fe atom at room temperature 1,4 and 1.89 B /Fe atom at 10 K. 5 The crystal structure is tetragonal space group I 4 ¯ ) with three different Fe sites denoted I, II, and III. The combination of a tetragonal structure and the intro- duction of P produces a large magnetocrystalline anisotropy. 6,7 The three different Fe sites have different mag- netic moments. At room temperature, neutron diffraction ex- periments revealed moments of 2.12, 1.25, and 1.83 B /atom, for site I, II, and III, respectively. 6 Interestingly, one can substitute for the Fe atoms, 3 d elements with addi- tional or less valence electrons, i.e., Cr, Mn, Co, and Ni, up to a certain limit, without changing the crystal structure. 4 This enables studies of the magnetic properties of one class of isostructural materials with the controlling parameter be- ing the filling of electrons in the valence band. Recently, a detailed experimental and theoretical study of the (Fe 1 -x Co x ) 3 P compounds 5 has been published, where it was found that the introduction of Co decreases the magnetic moment in the entire range of solid solution (0 x 0.37). The Co atoms were found to preferentially substitute Fe on atomic sites III and II. The magnetic properties of (Fe 1 -x Co x ) 3 P are well under- stood from a delocalized electron picture, with the 3 d elec- trons occupying band states, and it can be understood that the decreasing magnetic moment of the alloy as a function of Co concentration is due to a so called strong ferromagnetic or- dering. This means that the exchange splitting of the material is large so that additional valence electrons enter states of only one of the spin channels. In (Fe 1 -x Co x ) 3 P there are about 6.5–7.5 3 d electrons per metal atom depending on Co concentrationand consequently additional valence electrons provided by alloying of Co enter the spin down band causing a reduction of magnetic moment, which is consistent with observations. With this in mind one can speculate that re- placing Fe for Mn which has one less valence electron com- pared to Feshould increase the magnetic moment of the alloy due to the same band arguments. A decrease, on the other hand, would possibly reflect a different magnetic cou- pling between Mn and neighboring metal atoms Fe or Mn than ferromagnetic or alternatively a reduction of the ex- change splitting. PHYSICAL REVIEW B 1 JANUARY 2000-I VOLUME 61, NUMBER 1 PRB 61 0163-1829/2000/611/4139/$15.00 413 ©2000 The American Physical Society