The recent discovery of type-II multiferroicity in monolayer NiI2 indicated a new pathway for intrinsic magnetoelectric coupling in the two-dimensional limit. However, determining whether this phenomenon is a unique anomaly or a general, chemically tunable property of the material class remains unresolved.
Here, we demonstrate the universality of type-II multiferroicity in the transition metal dihalides by visualizing the ferroelectric order in monolayer NiBr2. Using scanning tunneling microscopy (STM), we resolve atomic-scale ferroelectric domains and confirm their magnetoelectric origin through reciprocal manipulation experiments: reorienting magnetic order via electric fields and suppressing the electric polarization with external magnetic fields.
Furthermore, we find that the multiferroic state in NiBr2 is energetically less robust than in its iodide counterpart, consistent with modified superexchange interactions and the reduced spin-orbit coupling.
Our results establish the transition metal dihalides as a versatile platform where the stability of magnetoelectric phases can be engineered through chemical substitution.