Ab initio study of the band structures of different phases of higher manganese silicides D. B. Migas,* V. L. Shaposhnikov, A. B. Filonov, and V. E. Borisenko Belarusian State University of Informatics and Radioelectronics, P.Browka 6, 220013 Minsk, Belarus N. N. Dorozhkin Belarusian State University, Nezavisimosti Av. 4, 220050 Minsk, Belarus Received 16 November 2007; revised manuscript received 14 January 2008; published 25 February 2008 By means of first principles calculations, we have investigated the band structures of different phases of higher manganese silicides MnSi x with x ranging from 1.73 to 1.75. In this family, Mn 11 Si 19 , Mn 15 Si 26 , and Mn 27 Si 47 have been found to behave like degenerate semiconductors and, at the same time, like metals because the Fermi level stays partly in the energy gap and partly in the valence band close to its top. The spin-polarized calculations have revealed that these phases can be also treated as half-metals displaying 100% spin polariza- tion of holes at the Fermi energy. On the contrary, Mn 4 Si 7 is shown to be a semiconductor with the indirect band gap of 0.77 eV. Its dielectric function possesses some anisotropy effects with respect to different light polarizations. We have also discovered that the MnSi 1.75 stoichiometry provides semiconductor properties without degeneracy. The role of stacking faults in the gap reduction of higher manganese silicides is discussed. DOI: 10.1103/PhysRevB.77.075205 PACS numbers: 71.20.Nr, 78.20.Bh, 75.50.Pp I. INTRODUCTION Semiconducting silicides have attracted much attention because of their prospects for optoelectronic and thermoelec- tric applications. 1 Among them, iron disilicide -FeSi 2 is one of the most promising and well studied both experimen- tally and theoretically. 1 However, in the case of higher man- ganese silicides HMSsMnSi x with x 1.73–1.75, also indicated to have promising properties, 1 there are several is- sues which are not fully understood and explored: the exis- tence of different phases with similar crystal structures and the value and the character of the gap in addition to the reported degenerate semiconducting nature and observed metallic behavior as a magnetic system. In fact, HMSs were shown to have several phases with slightly different stoichi- ometry see Table Isuch as Mn 4 Si 7 , 2 Mn 11 Si 19 , 3,4 Mn 15 Si 26 , 5 and Mn 27 Si 47 . 6 They all derived from the TiSi 2 structure 7 and displayed the tetragonal crystal structure with almost equal a lattice parameters and unusually long c lattice parameters Table I. The corresponding unit cells of HMSs are shown in Fig. 1. Moreover, HMSs are also characterized by the same building principle as determined by the high-resolution elec- tron microscopy study. 7 Thus, Mn atoms occupy Ti sites and form the Mn sublattice, while Si atoms in a double-helical arrangement form another sublattice by filling intersites in the Mn sublattice. A commensurate match of the two sublat- tices requires such a long c lattice parameter. However, it is hard to distinguish between different phases of HMS. 7,8 From the other side, resistivity of HMS indicates the be- havior usually observed for degenerate semiconductors: at temperatures below 500 K, the resistivity increases with temperature, while above 500 K, the resistivity starts de- creasing exponentially indicating the gap of about 0.4 eV. 9,10 The Hall effect measurements identify holes to be the domi- nant carriers in the whole temperature range, 911 and the hole mobility is shown to be very small. 811 The band gaps for bulk samples were found to scatter from 0.4 eV Ref. 9to 0.7 eV Ref. 11and to 0.9 eV. 12 In addition, the gaps of 0.40 and 0.42 eV have been obtained on thin film samples according to resistivity and the Hall effect experiments, respectively. 10 Bost and Mahan 13 by analyzing the absorption coefficient data have shown that polycrystalline films of HMS were characterized by the direct transition of 0.68 eV with a strong free carrier absorption below 0.2 eV. The same band gap was derived from their resistivity measurements. 13 Another optical investigation 14 carried out on a single layer of HMS has determined the direct band gap between 0.78 FIG. 1. Color onlineThe unit cells of HMS. The larger gray blueballs stand for Mn atoms, while the smaller dark redballs indicate Si atoms. PHYSICAL REVIEW B 77, 075205 2008 1098-0121/2008/777/0752059©2008 The American Physical Society 075205-1