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Register a new userCrafting the strain state in epitaxial thin films: A case study of CoFe2O4 films on Pb(Mg,Nb)O3-PbTiO3
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The strain dependence of electric and magnetic properties has been widely investigated, both from a fundamental science perspective and an applications point of view. Electromechanical coupling through field-induced polarization rotation (PRO) and polarization reorientation (PRE) in piezoelectric single crystals can provide an effective strain in film/substrate epitaxial heterostructures. However, the specific pathway of PRO and PRE is a complex thermodynamic process, depending on chemical composition, temperature, electric field and mechanical load. Here, systematic studies of the temperature-dependent field-induced phase transitions in Pb(Mg,Nb)O3-PbTiO3 single crystals with different initial phase and orientation configurations have been performed. Different types of strains, volatile/nonvolatile and biaxial/uniaxial, have been measured by both macroscopic and in-situ X-ray diffraction techniques. In addition, the strain state of epitaxial Mn-doped CoFe2O4 thin films was examined by magnetic anisotropy measurements, where a giant magnetoelectric coupling has been demonstrated.
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Ferroelectric switching and nanoscale domain dynamics were investigated using atomic force microscopy on monocrystalline Pb(Zr0.2Ti0.8)O3 thin films. Measurements of domain size versus writing time reveal a two-step domain growth mechanism, in which initial nucleation is followed by radial domain wall motion perpendicular to the polarization direction. The electric field dependence of the domain wall velocity demonstrates that domain wall motion in ferroelectric thin films is a creep process, with the critical exponent mu close to 1. The dimensionality of the films suggests that disorder is at the origin of the observed creep behavior.
Ferroelectric and dielectric properties of polydomain (twinned) single-crystal Pb(Zr1-xTix)O3 thin films are described with the aid of a nonlinear thermodynamic theory, which has been developed recently for epitaxial ferroelectric films with dense laminar domain structures. For Pb(Zr1-xTix)O3 (PZT) films with compositions x = 0.9, 0.8, 0.7, 0.6, 0.5, and 0.4, the misfit strain-temperature phase diagrams are calculated and compared with each other. It is found that the equilibrium diagrams of PZT films with x > 0.7 are similar to the diagram of PbTiO3 films. They consist of only four different stability ranges, which correspond to the paraelectric phase, single-domain tetragonal ferroelectric phase, and two pseudo-tetragonal domain patterns. In contrast, at x = 0.4, 0.5, and 0.6, the equilibrium diagram displays a rich variety of stable polarization states, involving at least one monoclinic polydomain state. Using the developed phase diagrams, the mean out-of-plane polarization of a poled PZT film is calculated as a function of the misfit strain and composition. Theoretical results are compared with the measured remanent polarizations of PZT films grown on SrTiO3. Dependence of the out-of-plane dielectric response of PZT films on the misfit strain in the heterostructure is also reported.
Epitaxial strain plays an important role in determining physical properties of perovskite ferroelectric oxide thin films. However, it is very challenging to directly measure properties such as polarization in ultrathin strained films using traditional sandwich capacitor devices, because of high leakage current. We employed a planar electrode device with different crystallographical orientations between electrodes along different electric field orientation to directly measure the in-plane polarization-electric field (P-E) hysteresis loops in fully strained thin films. At high misfit strains such as -4.4%, the pure Tetrogonal-like phase is obtained and its polarization vector is constrained to lie in the (010) plane with a significantly large in-plane component, ~44 {mu}C/cm2. First-principle calculations are carried out in parallel, and provide a good agreement with the experimental results. Our results pave the way to design in-plane devices based on T-like BFO and the strategy proposed here can be expanded to study all other similar strained multiferroic ultrathin films.
TbMnO$_{3}$ films have been grown under compressive strain on (001)-oriented SrTiO$_{3}$ crystals. They have an orthorhombic structure and display the (001) orientation. With increasing thickness, the structure evolves from a more symmetric (tetragonal) to a less symmetric (bulk-like orthorhombic) structure, while keeping constant the in-plane compression thereby leaving the out-of-plane lattice spacing unchanged. The domain microstructure of the films is also revealed, showing an increasing number of orthorhombic domains as the thickness is decreased: we directly observe ferroelastic domains as narrow as 4nm. The high density of domain walls may explain the induced ferromagnetism observed in the films, while both the decreased anisotropy and the small size of the domains could account for the absence of a ferroelectric spin spiral phase.
Berry curvature plays a crucial role in exotic electronic states of quantum materials, such as intrinsic anomalous Hall effect. As Berry curvature is highly sensitive to subtle changes of electronic band structures, it can be finely tuned via external stimulus. Here, we demonstrate in SrRuO3 thin films that both the magnitude and sign of anomalous Hall resistivity can be effectively controlled with epitaxial strain. Our first-principles calculations reveal that epitaxial strain induces an additional crystal field splitting and changes the order of Ru d orbital energies, which alters the Berry curvature and leads to the sign and magnitude change of anomalous Hall conductivity. Furthermore, we show that the rotation of Ru magnetic moment in real space of tensile strained sample can result in an exotic nonmonotonic change of anomalous Hall resistivity with the sweeping of magnetic field, resembling the topological Hall effect observed in non-coplanar spin systems. These findings not only deepen our understanding of anomalous Hall effect in SrRuO3 systems, but also provide an effective tuning knob to manipulate Berry curvature and related physical properties in a wide range of quantum materials.
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