Pressure-Tuned Intralayer Exchange in Superlattice-Like MnBi₂Te₄/(Bi₂Te₃) Topological Insulators

The magnetic structures of MnBi₂Te₄(Bi₂Te₃) can be manipulated by tuning the interlayer coupling via the number of Bi₂Te₃ spacer layers n, while the intralayer ferromagnetic (FM) exchange coupling is considered too robust to control. By applying hydrostatic pressure up to 3.5 GPa, we discover opposite responses of magnetic properties for n = 1 and 2. MnBi₄Te₇ stays at A-type antiferromagnetic (AFM) phase with a decreasing Néel temperature and an increasing saturation field. In sharp contrast, MnBi₆Te₁₀ experiences a phase transition from A-type AFM to a quasi-two-dimensional FM state with a suppressed saturation field under pressure. First-principles calculations reveal the essential role of intralayer exchange coupling from lattice compression in determining these magnetic properties. Such magnetic phase transition is also observed in 20% Sb-doped MnBi₆Te₁₀ because of the in-plane lattice compression.