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Oxygen vacancies (VO) effects on magnetic ordering in Eu0.5Ba0.5TiO3−δ (EBTO3−δ) thin films have been investigated using a combination of experimental measurements and first-principles density-functional calculations. Two kinds of EBTO3−δ thin films with different oxygen deficiency have been fabricated. A nuclear resonance backscattering spectrometry technique has been used to quantitatively measure contents of the VO. Eu0.5Ba0.5TiO3 ceramics have been known to exhibit ferroelectric (FE) and G-type antiferromagnetic (AFM) properties. While, a ferromagnetic (FM) behavior with a Curie temperature of 1.85 K has been found in the EBTO3−δ thin films. Spin-polarized Ti3+ ions, which originated from the VO, has been proven to mediate a FM coupling between the local Eu 4f spins and were believed to be responsible for the great change of the magnetic ordering. Considering the easy formation of VO, our work opens up a new avenue for achieving co-existence of FM and FE orders in oxide materials.

Oxygen-Vacancy-Induced Antiferromagnetism to Ferromagnetism Transformation in Eu0.5Ba0.5TiO3−δ Multiferroic Thin Films