Observation of the strain induced magnetic phase segregation of manganite thin films

Epitaxial strain alters the physical properties of thin films grown on single crystal substrates. Thin film oxides are particularly apt for strain engineering new functionalities in ferroic materials. In the case of La2/3Ca1/3MnO3 (LCMO) thin films, here we show the first experimental images obtained by electron holography demonstrating that epitaxial strain induces the segregation of a flat and uniform nonferromagnetic layer with antiferromagnetic (AFM) character at the top surface of a ferromagnetic (FM) layer, the whole film being chemical and structurally homogeneous at room temperature. For different substrates and growth conditions the tetragonality of LCMO at room temperature, defined as τ = |c – a|/a, is the driving force for a phase coexistence above an approximate critical value of τC ≈ 0.024. Theoretical calculations prove that the increased tetragonality changes the energy balance of the FM and AFM ground states in strained LCMO, enabling the formation of magnetically inhomogeneous states. This work gives the key evidence that opens a new route to synthesize strain-induced exchanged-biased FM–AFM bilayers in single thin films, which could serve as building blocks of future spintronic devices.This work was supported by Spanish Ministry of Science through projects No. MAT2011-28532-C03-02 and MAT2011-27553-C02 including FEDER funding, by the Aragon Regional Government through projects E26 and CTPP4/11, by the Universidad de Zaragoza through the contract PIF-UZ-2009-CIE-02, and by the European Union under the Seventh Framework Programme under a contract for an Integrated Infrastructure Initiative Reference 312483-ESTEEM2.Peer Reviewe