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Register a new userBuilt-in electric field induces polarization rotation in bilayer BiFeO3/(Ba,Sr)TiO3 thin films
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The crystal structure of BiFeO3/BaxSr1-xTiO3 (BFO/BST) heterostructures with x = 0.2, 0.6 and 0.8, grown on single-crystal MgO (001) substrate was investigated by x-ray diffraction and Raman spectroscopy in order to determine the influence of mismatch-induced strains and spontaneous polarization in BST buffer layers on BFO layers. The lattice parameter of the BFO layers was shown to decrease with increasing concentration of Ba ions, despite the increasing in-plain lattice parameters of tetragonal unit cells of BST layers. The rhombohedral angle of the crystal structure of BFO layers demonstrates an increase towards the ideal cubic perovskite structure with the appearance of the built-in electric field, induced by the spontaneous polarization in buffer layers. This result provides a remarkable tool for the control of polarization in BFO layers and other ferroelectric films in general, by changing the built-in electric field from ferroelectric buffer layer without changing a single crystal substrate.
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In this work we report on the controlled fabrication of a self-assembled line network in highly epitaxial BiFeO3 thin films on top of LaAlO3 in the kinetically limited grown region by RF sputtering. As previously shown in the case of manganite thin films, the remarkable degree of ordering is achieved using vicinal substrates with well-defined step-terrace morphology. Nanostructured BiFeO3 thin films show mixed-phase morphology. Besides typical formation following (100) and (010) axes, some mixed phase nanodomains are detected also in-between the regular line network. These particular microstructures open a playground for future applications in multiferroic nanomaterials.
We have studied electric-field-induced symmetry lowering in the tetragonal (001)-oriented heteroepitaxial (Ba$_{0.8}$Sr$_{0.2}$)TiO$_3$ thin film deposited on (001)MgO substrate. Polarized micro-Raman spectra were recorded from the film area in between two planar electrodes deposited on the film surface. Presence of textit{c}-domains with polarization normal to the substrate was confirmed from polarized Raman study under zero field, while splitting and hardening of the textit{E}(TO) soft mode and polarization changes in the Raman spectra suggest monoclinic symmetry under external electric field.
The emergent behaviors in thin films of a multiaxial ferroelectric due to an electrochemical coupling between the rotating polarization and surface ions are explored within the framework of the 2-4 Landau-Ginzburg-Devonshire (LGD) thermodynamic potential combined with the Stephenson-Highland (SH) approach. The combined LGD-SH approach allows to describe the electrochemical switching and rotation of polarization vector in the multiaxial ferroelectric film covered by surface ions with a charge density dependent to the relative partial oxygen pressure. We calculate the phase diagrams and analyze the dependence of polarization components on the applied voltage, and discuss the peculiarities of quasi-static ferroelectric, dielectric and piezoelectric hysteresis loops in thin strained multiaxial ferroelectric films. The nonlinear surface screening by oxygen ions makes the diagrams very different from the known diagrams of e.g., strained BaTiO3 films. Quite unexpectedly we predict the appearance of the ferroelectric reentrant phases. Obtained results point on the possibility to control the appearance and features of ferroelectric, dielectric and piezoelectric hysteresis in multiaxial FE films covered by surface ions by varying their concentration via the partial oxygen pressure. The LGD-SH description of a multiaxial FE film can be further implemented within the Bayesian optimization framework, opening the pathway towards predictive materials optimization.
A morphotropic phase boundary driven by epitaxial strain has been observed in a lead-free multiferroic BiFeO3 thin films and the strain-driven phase transitions were widely reported to be iso-symmetric Cc-Cc ones by recent works. In this paper, we suggest that the tetragonal-like BiFeO3 phase identified in epitaxial films on (001) LaAlO3 single crystal substrates is monoclinic MC. This MC phase is different from MA type monoclinic phase reported in BiFeO3 films grown on low mismatch substrates, such as SrTiO3. This is confirmed not only by synchrotron x-ray studies but also by piezoresponse force microscopy measurements. The polarization vectors of the tetragonal-like phase lie in the (100) plane, not the (110) plane as previously reported. A phenomenological analysis was proposed to explain the formation of MC Phase. Such a low symmetry MC phase, with its linkage to MA phase and the multiphase coexistence open an avenue for large piezoelectric response in BiFeO3 films and shed light on a complete understanding towards possible polarization rotation paths and enhanced multiferroicity in BiFeO3 films mediated by epitaxial strain. This work may also aid the understanding of developing new lead-free strain-driven morphotropic phase boundary in other ferroic systems.
The Landau theory of phase transitions of Ba0.8Sr0.2TiO3 thin film under external electric field applied in the planar geometry is developed. The interfacial van-der-Waals field Ez=1.1x10^8 V/m oriented normal to the film-substrate interface was introduced in to the model calculation to explain experimentally observed behavior of the polarization as a function of planar electric field. The Ez - misfit strain phase diagram of the film is constructed and discussed.
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