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Register a new userTemperature-driven evolution of hierarchical nanodomain structure in tetragonal-like BiFeO3 films
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Transmission electron microscopy study of tetragonal-like BiFeO3 films reveals a hitherto unreported hierarchical nanodomain structure. The 30-50 nm wide stripe domains with {110} domain walls consist of a substructure of lamellar nanodomains of 8-10 nm width in a herringbone-like arrangement. In situ heating and cooling reveals a reversible transition from the hierarchical nanodomain structure to a tweed-like domain structure which is accompanied by a first-order phase transition near 120 {deg}C with a thermal hysteresis.
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We have investigated the nanoscale switching properties of strain-engineered BiFeO3 thin films deposited on LaAlO3 substrates using a combination of scanning probe techniques. Polarized Raman spectral analysis indicate that the nearly-tetragonal films have monoclinic (Cc) rather than P4mm tetragonal symmetry. Through local switching-spectroscopy measurements and piezoresponse force microscopy we provide clear evidence of ferroelectric switching of the tetragonal phase but the polarization direction, and therefore its switching, deviates strongly from the expected (001) tetragonal axis. We also demonstrate a large and reversible, electrically-driven structural phase transition from the tetragonal to the rhombohedral polymorph in this material which is promising for a plethora of applications.
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.
We present a synchrotron grazing incidence x-ray diffraction analysis of the domain structure and polar symmetry of highly strained BiFeO3 thin films grown on LaAlO3 substrate. We revealed the existence of periodic elastic nanodomains in the pure tetragonal-like BFO ultrathin films down to a thickness of 6 nm. A unique shear strain accommodation mechanism is disclosed. We further demonstrated that the periodicity of the nanodomains increases with film thickness but deviates from the classical Kittels square root law in ultrathin thickness regime (6 - 30 nm). Temperature-dependent experiments also reveal the disappearance of periodic modulation above 90C due to a MC-MA structural phase transition.
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.
Defect engineering has been a powerful tool to enable the creation of exotic phases and the discovery of intriguing phenomena in ferroelectric oxides. However, accurate control the concentration of defects remains a big challenge. In this work, ion implantation, that can provide controllable point defects, allows us the ability to produce a controlled defect-driven true super-tetragonal (T) phase with enhanced tetragonality in ferroelectric BiFeO3 thin films. This point defect engineering is found to drive the phase transition from the as-grown mixed rhombohedral-like (R) and tetragonal-like (MC) phase to true tetragonal (T) symmetry. By further increasing the injected dose of He ion, we demonstrate an enhanced tetragonality super-tetragonal (super-T) phase with the largest c/a ratio (~ 1.3) that has ever been experimentally achieved in BiFeO3. A combination of morphology change and domain evolution further confirm that the mixed R/MC phase structure transforms to the single-domain-state true tetragonal phase. Moreover, the re-emergence of R phase and in-plane stripe nanodomains after heat treatment reveal the memory effect and reversible phase transition. Our findings demonstrate the control of R-Mc-T-super T symmetry changes and the creation of true T phase BiFeO3 with enhanced tetragonality through controllable defect engineering. This work also provides a pathway to generate large tetragonality (or c/a ratio) that could be extended to other ferroelectric material systems (such as PbTiO3, BaTiO3 and HfO2) which may lead to strong polarization enhancement.
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