Our neutron diffraction investigation of PrMn2Ge2−xSix reveals a clear separation into two magnetic phases, canted ferromagnetic (Fmc) and antiferromagnetic (AFmc), between x = 1.0 and 1.2 and a commensurate phase gap in the lattice, due to magnetostrictive distortion. This remarkable magnetoelastic phenomenon is driven by a nonuniform atomic distribution on the X site which in turn produces subtle variations in the local lattice and abrupt changes in the Mn-Mn magnetic exchange interaction. Our results show that coexistence of Fmc and AFmc phases depends on lattice parameter, chemical pressure from the rare-earth and metalloid sites, and local lattice strain distributions. We demonstrate that these magnetostructural correlations act across the entire family of R1−yRy′Mn2X2−xXx′ compounds.
ARC/DP0879070, ARC/DP110102386, ARC/LE0775559