No Arabic abstract
We show that misfit strain originated from the film-substrate lattice mismatch strongly increases the value of the quadratic magnetoelectric coupling. The giant magnetoelectric coupling, size effects and misfit strain cause strong changes of ferroic films phase diagrams at zero external magnetic and electric fields, in particular, the transformation of antiferromagnetic phase into ferromagnetic or ferrimagnetic ones for compressive or tensile misfit strains correspondingly as well as thickness induced paramagnetic or/and paraelectric phases appearance. Ferromagnetism appearance and magnetoelectric coupling increase in thin ferroelectric-antiferromagnetic films is in agreement with available experimental data and opens the way for tailoring of ferroic films magnetic and electric properties.
It is shown theoretically that a giant magnetoelectric susceptibility exceeding 10^-6 s/m may be achieved in the ferromagnetic/ferroelectric epitaxial systems via the magnetization rotation induced by an electric field applied to the substrate. The predicted magnetoelectric anomaly results from the strain-driven spin-reorientation transitions in ferromagnetic films, which take place at experimentally accessible misfit strains in CoFe2O4 and Ni films.
The coupling between ferroelectric and magnetic orders in multiferroic materials and the nature of magnetoelectric (ME) effects are enduring experimental challenges. In this work, we have studied the response of magnetization to ferroelectric switching in thin-film hexagonal YbFeO3, a prototypical improper multiferroic. The bulk ME decoupling and potential domain-wall ME coupling were revealed using x-ray magnetic circular dichroism (XMCD) measurements with in-situ ferroelectric polarization switching. Our Landau theory analysis suggests that the bulk ME-coupled ferroelectric switching path has a higher energy barrier than that of the ME-decoupled path; this extra barrier energy is also too high to be reduced by the magneto-static energy in the process of breaking single magnetic domains into multi-domains. In addition, the reduction of magnetization around the ferroelectric domain walls predicted by the Landau theory may induce the domain-wall ME coupling in which the magnetization is correlated with the density of ferroelectric domain walls. These results provide important experimental evidence and theoretical insights into the rich possibilities of ME couplings in hexagonal ferrites, such as manipulating the magnetic states by an electric field.
The effect of high tensile strain and low dimensionality on the magnetic and electronic properties of CaMnO$_3$ ultrathin films, epitaxially grown on SrTiO$_3$ substrates, are experimentally studied and theoretically analyzed. By means of ab initio calculations, we find that, both, the high strain produced by the substrate and the presence of the free surface contribute to the stabilization of an in-plane ferromagnetic coupling, giving rise to a non-zero net magnetic moment in the ultrathin films. Coupled with this change in the magnetic order we find an insulator-metal transition triggered by the quantum confinement and the tensile epitaxial strain. Accordingly, our magnetic measurements in 3nm ultrathin films show a ferromagnetic hysteresis loop, absent in the bulk compound due to its G-type antiferromagnetic structure.
Multiferroics are a unique class of materials where magnetic and ferroelectric orders coexist. The research on multiferroics contributes significantly to the fundamental understanding of the strong correlations between different material degrees of freedom and provides an energy-efficient route toward the electrical control of magnetism. While multiple ABO3 oxide perovskites have been identified as being multiferroic, their magnetoelectric coupling strength is often weak, necessitating the material search in different compounds. Here, we report the observation of room-temperature multiferroic orders in multi-anion SrNbO3-xNx thin films. In these samples, the multi-anion state enables the room-temperature ferromagnetic ordering of the Nb d-electrons. Simultaneously, we find ferroelectric responses that originate from the structural symmetry breaking associated with both the off-center displacements of Nb and the geometric displacements of Sr, depending on the relative O-N arrangements within the Nb-centered octahedra. Our findings not only diversify the available multiferroic material pool but also demonstrate a new multiferroism design strategy via multi-anion engineering.
It has been well established that both in bulk at ambient pressure and for films under modest strains, cubic SrCoO$_{3-delta}$ ($delta < 0.2$) is a ferromagnetic metal. Recent theoretical work, however, indicates that a magnetic phase transition to an antiferromagnetic structure could occur under large strain accompanied by a metal-insulator transition. We have observed a strain-induced ferromagnetic to antiferromagnetic phase transition in SrCoO$_{3-delta}$ films grown on DyScO$_3$ substrates, which provide a large tensile epitaxial strain, as compared to ferromagnetic films under lower tensile strain on SrTiO$_3$ substrates. Magnetometry results demonstrate the existence of antiferromagnetic spin correlations and neutron diffraction experiments provide a direct evidence for a G-type antiferromagnetic structure with Neel temperatures between $T_N sim 135,pm,10,K$ and $sim 325,pm,10,K$ depending on the oxygen content of the samples. Therefore, our data experimentally confirm the predicted strain-induced magnetic phase transition to an antiferromagnetic state for SrCoO$_{3-delta}$ thin films under large epitaxial strain.