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We report a Raman scattering investigation of multiferroic bismuth ferrite BiFeO3 epitaxial (c-axis oriented) thin films from -192 to 1000C. Phonon anomalies have been observed in three temperature regions: in the gamma-phase from 930C to 950C; at ~370C, Neel temperature (TN), and at ~123C, due to a phase transition of unknown type (magnetic or structural). An attempt has been made to understand the origin of the weak phonon-magnon coupling and the dynamics of the phase sequence. The disappearance of several Raman modes at ~820C (Tc) is compatible with the known structural phase transition and the Pbnm orthoferrite space group assigned by Arnold {it et al.} cite{arnold:09}. The spectra also revealed a {it non-cubic} $beta$-phase from 820-930dc and the same {it non-cubic} phase extends through the $gamma$-phase between 930-950dc, in agreement with Arnold {it et al.} cite{arnold2:09}, and an evidence of a cubic $delta$-phase around 1000dc in thin films that is not stable in powder and bulk. Such a cubic phase has been theoretically predicted in cite{vasquez:prb09}. Micro-Raman scattering and X-ray diffraction showed no structural decomposition in thin films during the thermal cycling from 22-1000dc.
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In multiferroic BiFeO3 thin films grown on highly mismatched LaAlO3 substrates, we reveal the coexistence of two differently distorted polymorphs that leads to striking features in the temperature dependence of the structural and multiferroic properties. Notably, the highly distorted phase quasi-concomitantly presents an abrupt structural change, transforms from a hard to a soft ferroelectric and transitions from antiferromagnetic to paramagnetic at 360+/-20 K. These coupled ferroic transitions just above room temperature hold promises of giant piezoelectric, magnetoelectric and piezomagnetic responses, with potential in many applications fields.
Crystal and domain structures of tensile-strained BiFeO3 films grown on orthorhombic (110)o PrScO3 substrates were investigated. All films possess a MB-type monoclinic structure with 109o stripe domains oriented along the [=i10]o direction. For films thicknesses less than ~40 nm, presence of well-ordered domains is proved by the detection of satellite peaks in synchrotron x-ray diffraction studies. For thicker films, For thicker films, only the Bragg reflections from tilted domains were detected. This is attributed to the broader domain size distribution in thicker films.Using planar electrodes,the in-plane polarization of the MB phase is determined to be 85 uC/cm2, which is much larger than that of compressive strained BiFeO3 films. Our results further reveal that the substrate monoclinic distortion plays a major role in determining the stripe domain formation of the rhombohedral ferroic epitaxial thin films, which sheds light to the understanding of elastic domain structure evolution in many other functional oxide thin films as well.
BiFeO3 thin films with various thicknesses were grown epitaxially on (001) LaSrAlO4 single crystal substrates using pulsed laser deposition. High resolution x-ray diffraction measurements revealed that a tetragonal-like phase with c-lattice constant ~4.65 {AA} is stabilized by a large misfit strain. Besides, a rhombohedral-like phase with c-lattice constant ~3.99 {AA} was also detected at film thickness of ~50 nm and above to relieve large misfit strains. In-plane piezoelectric force microscopy studies showed clear signals and self-assembled nanoscale stripe domain structure for the tetragonal-like regions. These findings suggest a complex picture of nanoscale domain patterns in BiFeO3 thin films subjected to large compressive strains.
We report a study on the thermodynamic stability and structure analysis of the epitaxial BiFeO3 (BFO) thin films grown on YAlO3 (YAO) substrate. First we observe a phase transition of MC-MA-T occurs in thin sample (<60 nm) with an utter tetragonal-like phase (denoted as MII here) with a large c/a ratio (~1.23). Specifically, MII phase transition process refers to the structural evolution from a monoclinic MC structure at room temperature to a monoclinic MA at higher temperature (150oC) and eventually to a presence of nearly tetragonal structure above 275oC. This phase transition is further confirmed by the piezoforce microscopy measurement, which shows the rotation of polarization axis during the phase transition. A systematic study on structural evolution with thickness to elucidate the impact of strain state is performed. We note that the YAO substrate can serve as a felicitous base for growing T-like BFO because this phase stably exists in very thick film. Thick BFO films grown on YAO substrate exhibit a typical morphotropic-phase-boundary-like feature with coexisting multiple phases (MII, MI, and R) and a periodic stripe-like topography. A discrepancy of arrayed stripe morphology in different direction on YAO substrate due to the anisotropic strain suggests a possibility to tune the MPB-like region. Our study provides more insights to understand the strain mediated phase co-existence in multiferroic BFO system.
We have combined neutron scattering and piezoresponse force microscopy to study the relation between the exchange bias observed in CoFeB/BiFeO3 heterostructures and the multiferroic domain structure of the BiFeO3 films. We show that the exchange field scales with the inverse of the ferroelectric and antiferromagnetic domain size, as expected from Malozemoffs model of exchange bias extended to multiferroics. Accordingly, polarized neutron reflectometry reveals the presence of uncompensated spins in the BiFeO3 film at the interface with the CoFeB. In view of these results we discuss possible strategies to switch the magnetization of a ferromagnet by an electric field using BiFeO3.
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