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Register a new userPolarization Instability in Polydomain Ferroelectric Epitaxial Thin Films and the Formation of Heterophase Structures
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Added by
Nicholas A. Pertsev
Publication date
1999
fields
Physics
and research's language is
English
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A thermodynamic theory is developed for dense laminar domain structures in epitaxial ferrolectric films. It is found that, at some critical misfit strain between the film and substrate, the 90 degrees c/a/c/a domain structure becomes unstable with respect to the appearance of the polarization component parallel to domain walls, which results in the formation of a heterophase structure. For PbTiO_3 and BaTiO_3 films, the stability ranges of polydomain and heterophase states are determined using misfit strain - temperature diagrams. Dielectric anomalies accompanying misfit-strain-driven structural transformations are described.
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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.
A Landau-Ginsburg-Devonshire-type nonlinear phenomenological theory is presented, which enables the thermodynamic description of dense laminar polydomain states in epitaxial ferroelectric thin films. The theory explicitly takes into account the mechanical substrate effect on the polarizations and lattice strains in dissimilar elastic domains (twins). Numerical calculations are performed for PbTiO3 and BaTiO3 films grown on (001)-oriented cubic substrates. The misfit strain-temperature phase diagrams are developed for these films, showing stability ranges of various possible polydomain and single-domain states. Three types of polarization instabilities are revealed for polydomain epitaxial ferroelectric films, which may lead to the formation of new polydomain states forbidden in bulk crystals. The total dielectric and piezoelectric small-signal responses of polydomain films are calculated, resulting from both the volume and domain-wall contributions. For BaTiO3 films, strong dielectric anomalies are predicted at room temperature near special values of the misfit strain.
We report on nanoscale strain gradients in ferroelectric HoMnO3 epitaxial thin films, resulting in a giant flexoelectric effect. Using grazing-incidence in-plane X-ray diffraction, we measured strain gradients in the films, which were 6 or 7 orders of magnitude larger than typical values reported for bulk oxides. The combination of transmission electron microscopy, electrical measurements, and electrostatic calculations showed that flexoelectricity provides a means of tuning the physical properties of ferroelectric epitaxial thin films, such as domain configurations and hysteresis curves.
Ferroelectric BaTiO3 films with large polarization have been integrated with Si(001) by pulsed laser deposition. High quality c-oriented epitaxial films are obtained in a substrate temperature range of about 300 deg C wide. The deposition temperature critically affects the growth kinetics and thermodynamics balance, resulting on a high impact in the strain of the BaTiO3 polar axis, which can exceed 2% in films thicker than 100 nm. The ferroelectric polarization scales with the strain and therefore deposition temperature can be used as an efficient tool to tailor ferroelectric polarization. The developed strategy overcomes the main limitations of the conventional strain engineering methodologies based on substrate selection: it can be applied to films on specific substrates including Si(001) and perovskites, and it is not restricted to ultrathin films.
Doping ferroelectric Hf0.5Zr0.5O2 with La is a promising route to improve endurance. However, the beneficial effect of La on the endurance of polycrystalline films may be accompanied by degradation of the retention. We have investigated the endurance - retention dilemma in La-doped epitaxial films. Compared to undoped epitaxial films, large values of polarization are obtained in a wider thickness range, whereas the coercive fields are similar, and the leakage current is substantially reduced. Compared to polycrystalline La-doped films, epitaxial La-doped films show more fatigue but there is not significant wake-up effect and endurance-retention dilemma. The persistent wake-up effect common to polycrystalline La-doped Hf0.5Zr0.5O2 films, is limited to a few cycles in epitaxial films. Despite fatigue, endurance in epitaxial La-doped films is more than 1010 cycles, and this good property is accompanied by excellent retention of more than 10 years. These results demonstrate that wake-up effect and endurance-retention dilemma are not intrinsic in La-doped Hf0.5Zr0.5O2.
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