We present the temperature- and thickness-dependent structural and morphological evolution of strain induced transformations in highly-strained epitaxial BiFeO3 films deposited on LaAlO3 (001) substrates. Using high-resolution X-ray diffraction and temperature-dependent scanning-probe-based studies we observe a complex temperature- and thickness-dependent evolution of phases in this system. A thickness-dependent transformation from a single monoclinically distorted tetragonal-like phase to a complex mixed-phase structure in films with thicknesses up to ~200 nm is the consequence of a strain-induced spinodal instability in the BiFeO3/LaAlO3 system. Additionally, a breakdown of this strain-stabilized metastable mixed-phase structure to non-epitaxial microcrystals of the parent rhombohedral structure of BiFeO3 is observed to occur at a critical thickness of ~300 nm. We further propose a mechanism for this abrupt breakdown that provides insight into the competing nature of the phases in this system.
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.
The novel strain-driven morphotropic phase boundary (MPB) in highly-strained BiFeO3 thin film is featured by ordered mixed phase nanodomains (MPNs). Through scanning probe microscopy and synchrotron X-ray diffraction, eight structural variants of the MPNs are identified. Detailed polarization configurations within the MPNs are resolved using angular-dependent piezoelectric force microscopy. Guided by the obtained results, deterministic manipulation of the MPNs has been demonstrated by controlling the motion of the local probe. These findings are important for in-depth understanding of the ultrahigh electromechanical response arising from phase transformation between competing phases, enabling future explorations on the electronic structure, magnetoelectricity and other functionalities in this new MPB system.
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.
The nanostructural evolution of the strain-induced structural phase transition in BiFeO3 is examined. Using high-resolution X-ray diffraction and scanning-probe microscopy-based studies we have uniquely identified and examined the numerous phases present at these phase boundaries and have discovered an intermediate monoclinic phase in addition to the previously observed rhombohedral- and tetragonal-like phases. Further analysis has determined that the so-called mixed-phase regions of these films are not mixtures of rhombohedral- and tetragonal-like phases, but intimate mixtures of highly-distorted monoclinic phases with no evidence for the presence of the rhombohedral-like parent phase. Finally, we propose a mechanism for the enhanced electromechanical response in these films including how these phases interact at the nanoscale to produce large surface strains.
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.
Anoop R. Damodaran
,Sungki Lee
,Karthik Jambunathan
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(2011)
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"Temperature and thickness evolution and epitaxial breakdown in highly-strained BiFeO3 thin films"
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Lane Martin Lane Martin
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