Chemical Manipulation of Magnetic Ordering in Mn1-xSnxBi2Se4 Solid-Solutions

Pierre Ferdinand P. Poudeu

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Kulugammana GS Ranmohotti, Honore Djieutedjeu, and Pierre FP Poudeu (2012)

Journal of the American Chemical Society, 134(34):14033-14042.

Several compositions of manganese tin bismuth selenide solid solution series, Mn1-xSnxBi2Se4 (x = 0, 0.3, 0.75), were synthesized by combining high purity elements in the desired ratio at moderate temperatures. X-ray single crystal studies of a Mn-rich composition (x = 0) and a Mn-poor phase (x = 0.75) at 100 and 300 K revealed that the compounds crystallize isostructurally in the monoclinic space group C2/m (no.12) and adopt the MnSb2Se4 structure type. Direct current (DC) magnetic susceptibility measurements in the temperature range from 2 to 300 K indicated that the dominant magnetic ordering within the Mn1-xSnxBi2Se4 solid-solutions below SO K switches from antiferromagnetic (AFM) for MnBi2Se4 (x = 0), to ferromagnetic (FM) for Mn0.7Sn0.3Bi2Se4 (x = 0.3), and finally to paramagnetic (PM) for Mn0.25Sn0.75Bi2Se4 (x = 0.75). We show that this striking variation in the nature of magnetic ordering within the Mn1-xSnxBi2Se4 solid-solution series can be rationalized by taking into account: (1) changes in the distribution of magnetic centers within the structure arising from the Mn to Sn substitutions, (2) the contributions of spin-polarized free charge carriers resulting from the intermixing of Mn and Sn within the same crystallographic site, and (3) a possible long-range ordering of Mn and Sn atoms within individual M(n)Se4n+2 single chain leading to quasi isolated MnSe6 octahedra spaced by nonmagnetic SnSe6 octahedra.

Times Cited: 2

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