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Register a new userEpitaxial growth and magnetoelectric relaxor behavior in multiferroic 0.8Pb(Fe1/2Nb1/2)O3-0.2Pb(Mg1/2W1/2)O3 thin films
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Wei Peng
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We present electric and magnetic properties of 0.8Pb(Fe1/2Nb1/2)O3-0.2Pb(Mg1/2W1/2)O3 films epitaxially grown on (001) SrTiO3 substrates using pulsed laser deposition. A narrow deposition window around 710 oC and 0.2 mbar has been identified to achieve epitaxial single-phase thin films. A typical Vogel-Fulcher relaxor-like dielectric and magnetic susceptibility dispersion is observed, suggesting magnetoelectric relaxor behavior in these films similar to the bulk. We determine a magnetic cluster freezing temperature of 36 K, while observing weak ferromagnetism via magnetic hysteresis loops up to 300 K.
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Single crystals of Pb(In1/2Nb1/2)O3-Pb(Mg1/3Nb2/3)O3-PbTiO3 (PIN-PMN-PT) poled along [001] were investigated by dielectric, x-ray, and polarized light (PLM) and piezo-force microscopy (PFM) methods. PLM revealed {100} macro-domain plates that formed after poling, whose size increased on heating between room temperature and a rhombohedral rightarrow tetragonal phase transition, above which point a break-up of the macro-domain plates was observed. Corresponding PFM studies demonstrated that poling reduced the size of stripe-like domains that were internal to the macro-domain plates, whose size also increased on heating to TR-T. The temperature dependence of both the size of the macro-domain plates and internal sub-domains followed the Arrhenius relation with the activation energy of 0.4-0.5eV. The coercive field displays an abnormal increase on heating below TR-T, different than that for PMN-PT. The anomalously increased coercive field can be ascribed to the Arrhenius-type domain growth, indicating a simple thermally activated process and an important role of hierarchial domains in the improved performance of PIN-PMN-PT.
The existence of polar nanoregions is the most important characteristic of ferroelectric relaxors, however, the size determination and dynamic of PNRs remains uncertain. We reveal a re-entrant relaxor behavior and ferroelectric-paraelectric transition coexists in complex perovskite oxide 0.6Bi(Mg1/2Ti1/2)O3-0.4PbTiO3. Two dielectric anomalies (i) the low-temperature re-entrant relaxor transition and (ii) the high-temperature diffuse phase transition (DPT) were described by the phenomenological statistical model. The sizes of the two kinds of polar nanoregions (PNRs) corresponding to two ferroelectric states were obtained. The dynamic of PNRs were analyzed using isothermal electrical modulus, which shows three critical temperatures associated with the diffuse phase transition, the formation and freezing of PNRs, respectively. The temperature evolution of the PNRs evolution depends on the stoichiometry of bismuth. The results provide new insights into the dynamic behavior of PNRs and the modification way of re-entrant relaxor behavior.
The electronic valence state of Mn in Pb(Zr0.2Ti0.8)O3/La0.8Sr0.2MnO3 multiferroic heterostructures is probed by near edge x-ray absorption spectroscopy as a function of the ferroelectric polarization. We observe a temperature independent shift in the absorption edge of Mn associated with a change in valency induced by charge carrier modulation in the La0.8Sr0.2MnO3, demonstrating the electronic origin of the magnetoelectric effect. Spectroscopic, magnetic, and electric characterization shows that the large magnetoelectric response originates from a modified interfacial spin configuration, opening a new pathway to the electronic control of spin in complex oxide materials.
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.
Ferroelectric switching and nanoscale domain dynamics were investigated using atomic force microscopy on monocrystalline Pb(Zr0.2Ti0.8)O3 thin films. Measurements of domain size versus writing time reveal a two-step domain growth mechanism, in which initial nucleation is followed by radial domain wall motion perpendicular to the polarization direction. The electric field dependence of the domain wall velocity demonstrates that domain wall motion in ferroelectric thin films is a creep process, with the critical exponent mu close to 1. The dimensionality of the films suggests that disorder is at the origin of the observed creep behavior.
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