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Register a new userNon-equilibrium Strain Relaxation Noise in the Relaxor Ferroelectric (PbMg1/3Nb2/3O3)100-x( PbTiO3)x
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Added by
Michael B. Weissman
Publication date
2018
fields
Physics
and research's language is
English
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Large low-frequency noise is found in some perovskite relaxor ferreoelectrics when they are polarized, regardless of whether the polarization is accompanied by an applied electric field. The noise appears both in the ferroelectric and relaxor states, including in the nominally ergodic paraelectric state at temperatures above the susceptibility peak. Since it is present whenever the samples are microphonic due to piezoelectricity but not evident when they are not microphonic, it appears to be a response to mechanical strain changes. Dependence of the noise on sample thermal history indicates that non-equilibrium strain relaxation is the source, even in the temperature range for which the sample is nominally ergodic. Non-equilibrium noise in the absence of net piezoelectricity is found at somewhat higher frequencies.
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The relaxor ferroelectric PbMg1/Nb2/3O3 was investigated by means of broad-band dielectric and Fourier Transform Infrared (FTIR) transmission spectroscopy in the frequency range from 1 MHz to 15 THz at temperatures between 20 and 900 K using PMN films on infrared transparent sapphire substrates. While thin film relaxors display reduced dielectric permittivity at low frequencies, their high frequency intrinsic or lattice response is shown to be the same as single crystal/ceramic specemins. It was observed that in contrast to the results of inelastic neutron scattering, the optic soft mode was underdamped at all temperatures. On heating, the TO1 soft phonon followed the Cochran law with an extrapolated critical temperature equal to the Burns temperature of 670 K and softened down to 50 cm-1. Above 450 K the soft mode frequency leveled off and slightly increased above the Burns temperature. A central mode, describing the dynamics of polar nanoclusters appeared below the Burns temperature at frequencies near the optic soft mode and dramatically slowed down below 1 MHz on cooling below room temperature. It broadened on cooling, giving rise to frequency independent losses in microwave and lower frequency range below the freezing temperature of 200 K. In addition, a new heavily damped mode appeared in the FTIR spectra below the soft mode frequency at room temperature and below. The origin of this mode as well as the discrepancy between the soft mode damping in neutron and infrared spectra is discussed.
We report lattice dynamical measurements, made using neutron inelastic scattering methods, of the relaxor perovskite PbMg1/3Nb2/3O3 (PMN) at momentum transfers near the edge of the Brillouin zone. Unusualcolumns of phonon scattering that are localized in momentum, but extended in energy, are seen at both high-symmetry points along the zone edge: vec{Q}_R={1/2, 1/2, 1/2} and vec{Q}_M={1/2,1/2,0}. These columns soften at ~400 K which is similar to the onset temperature of the zone-center diffuse scattering, indicating a competition between ferroelectric and antiferroelectric distortions. We propose a model for the atomic displacements associated with these phonon modes that is based on a combination of structure factors and group theoretical analysis. This analysis suggests that the scattering is not from tilt modes (rotational modes of oxygen octahedra), but from zone-boundary optic modes that are associated with the displacement of Pb^{2+} and O^{2-} ions. Whereas similar columns of scattering have been reported in metallic and (less commonly) molecular systems, they are unusual in insulating materials, particularly in ferroelectrics; therefore, the physical origin of this inelastic feature in PMN is unknown. We speculate that the underlying disorder contributes to this unique anomaly.
We report first principles density functional calculations of the Born effective charges and electronic dielectric tensors for the relaxor PMN (PbMg1/3Nb2/3O3). Visualization of the Born charge tensors as charge ellipsoids have provided microscopic insights on the factors governing piezoelectric enhancements with polarization rotation. Several 15 and 30-atom ferroelectric and antiferroelectric supercells of PMN involving 1:2 and 1:1 chemical ordering have been studied. A cascading set of ferroelectric phonon instabilities lead to several low symmetry monoclinic structures. We find a ground state with a 15-atom unit cell with 1:2 chemical ordering along [111] with a monoclinic C2 structure.
Structural phase transformations in (001)-oriented (1-x)Pb(Mg1/3Nb2/3O3)-32%PbTiO3 (PMN-x%PT) crystals have been investigated by x-ray diffraction. A C->T->MC sequence was observed in both the field-cooled (FC) and zero-field-cooled (ZFC) conditions. Most interestingly, an anomalous increase in the C->T phase boundary with increasing field has been observed, which is seemingly a common characteristic of crystals whose compositions are in the vicinity of the MPB, irrespective of the width of the T and MC phase regions.
A new class of superparamagnetism was found in relaxor ferroelectric 2/3BiFeO$_{3}$-1/3BaTiO$_{3}$. The size of the magnetic particle, estimated from the superparamagnetic magnetization curve, coincides with the size of the polar nanoregion (PNR), which governs the relaxor ferroelectric property. This suggests that the magnetic domain is identical to the PNR. The temperature variations in the sizes of the magnetic domains and PNRs estimated by our neutron diffraction measurements support this picture. Since the same domain provides both electric and magnetic properties, strong coupling between the two properties through the domain size is expected.
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