Theoretical evidence and chemical origin of the magnetism-dependent electrostructural coupling in La2NiMnO6

Using first-principles density-functional calculations, we determine and analyze the Born effective charges Z(*) that describe the coupling between electric field and atomic displacements for ferromagnetic double-perovskite compound, La2NiMnO6. We find that th Born effective charge matrix of Ni in La2NiMnO6, has an anomalously large antisymmetric component, whose magnitude reduces substantially upon change in the magnetic ordering between Ni and Mn, showing it to be a magnetism-dependent electrostructural coupling. We use a local picture of the electronic structure obtained with Wannier functions, along with its band-by-band decomposition to determine its electronic origin.