We investigate the magnetic and transport evolution in Mn3+xGa1−xC (0≤x≤0.60), where Mn substitution at corner Ga sites induces lattice contraction and suppresses the antiferromagnetic order of Mn3GaC. As x increases, the magnetic ground state of the system undergoes a sequential transition from an antiferromagnetic state, via a canted ferrimagnetic state, to a robust ferrimagnetic state, accompanied by a surge in the magnetic ordering temperature. Saturation magnetic moments reaches a maximum of 3.63~μB/f.u. at x=0.10, whereas the topological Hall resistivity peaks at 1.47~μΩ⋅cm for x=0.20 before decreasing with further doping. First-principles calculations demonstrate a ∼40∘ canting of face-centered Mn moments at x=0.20, signifying spin frustration, and an eventual antiparallel alignment of face-centered and corner-site Mn moments at higher x. These results reveal that intersublattice antiferromagnetic coupling governs the magnetic transformation and emergent transport phenomena, thus providing a microscopic foundation for designing high-ordering-temperature antiperovskites.
@article{arxiv.2603.24185,
title = {Tunable intersublattice exchange coupling drives magnetic evolution in Mn$_{3+x}$Ga$_{1-x}$C ($0 \le x \le 0.60$)},
author = {Dong-Hui Xu and Cong-Mian Zhen and Deng-Lu Hou and Li Ma and De-Wei Zhao and Guo-ke Li},
journal= {arXiv preprint arXiv:2603.24185},
year = {2026}
}