The study of magnetoelectric materials has recently received renewed interest, in large part stimulated by breakthroughs in the controlled growth of complex materials and by the search for novel materials with functionalities suitable for next generation electronic devices. In this Progress Report, we present an overview of recent developments in the field, with emphasis on magnetoelectric coupling effects in complex oxide multiferroic composite materials.

Magnetoelectric coupling effects in multiferroic complex oxide composite structures.

Magnetoelectric Coupling Effects in Multiferroic Complex Oxide Composite Structures

The magnetization $(M)$ of a ${\text{LaCoO}}_{3}$ film grown epitaxially on a piezoelectric substrate has been investigated in dependence on the biaxial in-plane strain. $M$ decreases with the reversible release of tensile strain, with a maximum change of at least 6% per 0.1% of biaxial strain near the Curie temperature $({T}_{C})$. The biaxial strain response of ${T}_{C}$ is estimated to be below 5 K/% in the tensile strain state. This is in agreement with results from statically strained films on various substrates. As possible origins of the strain-induced magnetization are considered (i) the strain-dependent Curie temperature, (ii) a strain-dependent magnetically inhomogeneous (phase-separated) state, and (iii) a strain-dependent magnetic moment (spin state) of Co ions. The ${T}_{C}$ shift is found insufficient to explain the measured strain-induced magnetization change but contributions from mechanism (ii) or (iii) must be involved.

Reversible strain effect on the magnetization of LaCoO 3 films

The crystalline and defect structure of epitaxial hexagonal RExMnyO3 (RE = Er, Dy) films with varying cationic composition was investigated by X-ray diffraction and transmission electron microscopy. The films are composed of a strained layer at the interface with the substrate and of a relaxed layer on top of it. The critical thickness is of ∼10 to 25 nm. For Mn-rich films (or RE deficient), an off-stoichiometric composition maintaining the hexagonal LuMnO3-type structure is stabilized over a large range of the RE/Mn ratio (0.72−1.00), with no Mn-rich secondary phases observed. A linear dependence of the out-of-plane lattice parameter with RE/Mn is observed in this range. Out-of-phase boundary (OPB) extended defects are observed in all films and exhibit a local change in stoichiometry. Such a large solubility limit in the RE deficient region points toward the formation of vacancies on the RE site (RExMnO3−δ, with 0.72 ≤ x < 1), a phenomenon that is encountered in perovskite manganites such as LaxMnO3−δ (x...

Off-Stoichiometry Effects on the Crystalline and Defect Structure of Hexagonal Manganite REMnO3 Films (RE = Y, Er, Dy)

Phase separation into a ferromagnetic (FM) metallic and a charge-ordered (CO) insulating state as found in the manganite ${({\text{Pr}}_{1\ensuremath{-}y}{\text{La}}_{y})}_{0.7}{\text{Ca}}_{0.3}{\text{MnO}}_{3}$ (PLCMO) is expected to be sensitive to structural changes. Reversible biaxial strain has been applied to epitaxially grown films on piezoelectric substrates of ${({\text{PbMg}}_{1/3}{\text{Nb}}_{2/3}{\text{O}}_{3})}_{0.72}{({\text{PbTiO}}_{3})}_{0.28}$ (001). Reversible strain experiments give a unique insight into the effect of strain on the magnetization and the electrical resistance, i.e., the so-called elastoresistance, of the films. 100-nm-thick PLCMO films of various Pr/La ratios have been grown using alternating pulsed laser deposition from a La-based and a Pr-based target. We have found a drastic reduction in the resistance, or a ``colossal'' elastoresistance, upon piezoelectrically controlled release of the tensile strain in the films, characterized by a resistive gauge factor of up to 1800. This result is qualitatively consistent with the magnetic measurements, where a higher saturation magnetization and an increased magnetic transition temperature are observed with the release of tensile strain. The elastoresistance is highest at chemical composition $y\ensuremath{\approx}0.6$, the metal-insulator phase boundary, and near the metal-insulator transition temperature, where the competition between the FM and CO ground states is strongest. This indicates that the coexistence of the FM and CO phases is strongly affected by strain with tensile strain suppressing the FM metallic phase.

Colossal elastoresistance and strain-dependent magnetization of phase-separated (Pr 1-y La y ) 0.7 Ca 0.3 MnO 3 thin films

We discuss three different approaches towards ferroelectric control of thin film magnetism and recent experimental results. Firstly, ferromagnetic films of doped LaMnO3 were grown on piezoelectric Pb(Mg1/3Nb2/3)0.72Ti0.28O3(001) crystals and have been strained reversibly by up to 0.15%. The strain modulation is accompanied by large magnetization changes (for example, of 25% at ambient temperature in La0.7Sr0.3MnO3), strong resistance modulations and a shift of the magnetic Curie temperature. Secondly, the concept of a multiferroic field-effect transistor comprising a magnetic channel and a ferroelectric gate is introduced. We discuss the effect of piezoelectric gate strain. Finally, the first results on single-phase multiferroic films of HoMnO3 are described. Epitaxial films have been prepared by the pulsed laser deposition technique. †We would like to devote this article to Prof. Hartmut Fues on the occasion of his official retirement. He has been active in the area of structural research on oxides throu...

Approaches towards ferroelectric control of thin film magnetism

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Approaches towards ferroelectric control of thin film magnetism