By means of first-principles calculations, the two-dimensional magnetic metal–organic framework, manganese phthalocyanine (MnPc), is proposed to exhibit nearly zero Poisson’s ratio within the elastic regime. Negative Poisson’s ratio can be reached by further increasing the uniaxial tensile strain beyond the yield point. Such an unusual mechanical property is found to rely on the spin-state of Mn atoms. Without strain, the ground state is ferrimagnetic and half-metallic. Interestingly, as the interatomic distance between Mn atoms increases under biaxial tensile strain, the alignment of magnetic moments of neighboring Mn atoms changes from antiparallel to parallel, associated with oscillatory exchange coupling strength. This not only reveals the strain-induced magnetic phase transition, but also indicates the magnetic interaction is mediated by the Ruderman–Kittel–Kasuya–Yosida exchange coupling and thus Kondo effect is likely to exist. Rather than the reported RKKY exchange coupling between supramolecular MnPc adsorbed on substrates, the predicted RKKY exchange coupling here exists in the pristine two-dimensional MnPc lattice. It would be more suitable for device applications because of the reduced size. Besides, it is noted that neighboring Mn atoms with antiparallel magnetic moments are responsible for the conducting behaviors, while those with parallel magnetic moments obstruct the flow of electrons. This property provides possibility of molding the flow of fully spin-polarized electrons through the manipulation of local magnetization by an external magnetic field, which is an attractive magnetoelectric response: the magnetic-field-controlled electron flow.
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