Near-room temperature ferromagnetic behavior of single-atom-thick 2D iron in nanolaminated ternary MAX phases

Mn+1AXn (MAX) phases' nanolaminated ternary carbides or nitrides possess a unique crystal structure in which single-atom-thick “A” sublayers are interleaved by alternative stacking of a “Mn+1Xn” sublayer; these materials have been investigated as promising high-safety structural materials for industrial applications because of their laminated structure and metal and ceramic properties. However, limited of A-site elements in the definition of Mn+1AXn phases, it is a huge challenge for designing nanolaminated ferromagnetic materials with single-atom-thick two-dimensional iron layers occupying the A layers in the Mn+1AXn phases. Here, we report three new ternary magnetic Mn+1AXn phases (Ta2FeC, Ti2FeN, and Nb2FeC) with A sublayers of single-atom-thick two-dimensional iron through an isomorphous replacement reaction of Mn+1AXn precursors (Ta2AlC, Ti2AlN, and Nb2AlC) with a Lewis acid salts (FeCl2). All these Mn+1AXn phases exhibit ferromagnetic behavior. The Curie temperatures of the Ta2FeC and Nb2FeC Mn+1AXn phases are 281 and 291 K, respectively, i.e., close to room temperature. The saturation magnetization of these ternary magnetic MAX phases is almost two orders of magnitude higher than V2(Sn,Fe)C, whose A-site is partially substituted by Fe. Theoretical calculations on magnetic orderings of spin moments of Fe atoms in these nanolaminated magnetic Mn+1AXn phases reveal that the magnetism can be mainly ascribed to an intralayer exchange interaction of the two-dimensional Fe atomic layers. Owing to the richness in composition of Mn+1AXn phases, our work provides a large imaginary space for constructing functional single-atom-thick two-dimensional layers in materials using these nanolaminated templates.