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We study the origin of the magnetoelectric coupling in manganite films on ferroelectric substrates. We find large magnetoelectric coupling in La 0.7 Ca 0.3 MnO 3 /BaTiO 3  ultra-thin films in experiments based on the converse magnetoelectric effect. The magnetization changes by around 30–40% upon applying electric fields on the order of 1 kV/cm to the BaTiO 3  substrate, corresponding to magnetoelectric coupling constants on the order of α = (2–5)·10 −7  s/m. Magnetic anisotropy is also affected by the electric field induced strain, resulting in a considerable reduction of coercive fields. We compare the magnetoelectric effect in pre-poled and unpoled BaTiO 3  substrates. Polarized neutron reflectometry reveals a two-layer behavior with a depressed magnetic layer of around 30 Å at the interface. Magnetic force microscopy (MFM) shows a granular magnetic structure of the La 0.7 Ca 0.3 MnO 3 . The magnetic granularity of the La 0.7 Ca 0.3 MnO 3  film and the robust magnetoelastic coupling at the La 0.7 Ca 0.3 MnO 3 /BaTiO 3  interface are at the origin of the large magnetoelectric coupling, which is enhanced by phase separation in the manganite.

Phase separation enhanced magneto-electric coupling in La0.7Ca0.3MnO3/BaTiO3 ultra-thin films