A spin Mn3d5–rich Mn60Bi40 alloy reveals a model system in order to tailor profound magnetic properties at unpaired 3d5 spins in such alloys of a core-shell structure. As annealed (at a critical temperature 573 K in H2 gas), a refined powder (in glycine) grows on α-MnBi seeds (crystallites) present in it at Mn/Bi atoms order over topological layers, preferentially along (110) planes, at a self-confined structure at seeds of an anisotropic shape of hexagonal (h) plates (25 to 85 nm widths). In terms of the HRTEM images, the atoms turn down at edges (at the plates grow up) in a spiral layer, ≤ 2.1 nm thickness, of small core-shells. A spin model is proposed to delineate a way at the spins can pin down at the edges, form single magnetic domains, and raise coercivity (Hc), with no much loss of net magnetic moment. The X-ray diffraction and HRTEM images corroborate the results of topological pacing of atoms at the h-plates at anneals. A novelty is that a core-shell leads to tailor a superb Hc, as much as 11.110 kOe (16.370 kOe at 350 K), with a fairly large magnetization, 76.5 emu/g, at near 300 K. An enhanced Curie point 650.1 K (628 K at Mn50Bi50 alloy) confers a surplus 3d5-Mn spin sensitively tunes α-MnBi stoichiometry and so its final magnetic structure. A refined alloy powder so made is useful to make powerful magnets and devices in the forms of films and bonded magnets in different shapes for uses as small tools, tweezers, and other devices.

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The MnBi alloys is a model series of rare-earth free magnets for surge of technologies of small parts of automobiles, power generators, medical tools, memory systems, and many others. The magnetics stem primarily at unpaired Mn-3d5 spins (a 4.23 B moment) align parallel via an orbital moment 0.27 B of Bi-5d106s2p3 in a crystal lattice. Thus, using a surplus Mn (over Bi) in a Mn70Bi30 type alloy designs a spin-rich system of duly tailored properties useful for magnetics and other devices. In this view, we report here a strategy of a refined alloy powder Mn70Bi30 can grow into small crystals of hexagonal (h) plates at seeds as annealed in magnetic fields (in H2 gas). So, small h-plates (30 to 50 nm widths) are grown up at (002) facets, wherein the edges are turned down in a spiral ( 2.1 nm thicknesses) in a core-shell structure. The results are described with X-ray diffraction, lattice images and magnetic properties of a powder Mn70Bi30 (milled in glycine) is annealed at 573 K for different time periods, so to the Mn/Bi order at the permeable facets (seeds). Duly annealed samples exhibit an enhanced magnetization, Ms  70.8 emu/g, with duly promoted coercivity Hc  10.810 kOe (15.910 kOe at 350 K), energy–product 14.8 MGOe, and the crystal-field-anisotropy, K1  7.6x107 erg/cm3, reported at room temperature. Otherwise, Ms should decline at any surplus 3d5-Mn spins order antiparallel at the antisites. Enhanced Curie point 658.1 K (628 K at Mn50Bi50 alloy) anticipates that a surplus Mn does favor the Mn-Bi exchange interactions. Proposed spin models well describe the spin-dynamics and lattice relaxations (on anneals) over the lattice volume (with twins) and spin clusters.