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Register a new userCoexistence and competition of local- and long-range polar orders in a ferroelectric relaxor
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We have performed a series of neutron diffuse scattering measurements on a single crystal of the solid solution Pb(Zn$_{1/3}$Nb$_{2/3}$)O$_3$ (PZN) doped with 8% PbTiO$_3$ (PT), a relaxor compound with a Curie temperature T$_C sim 450$ K, in an effort to study the change in local polar orders from the polar nanoregions (PNR) when the material enters the ferroelectric phase. The diffuse scattering intensity increases monotonically upon cooling in zero field, while the rate of increase varies dramatically around different Bragg peaks. These results can be explained by assuming that corresponding changes occur in the ratio of the optic and acoustic components of the atomic displacements within the PNR. Cooling in the presence of a modest electric field $vec{E}$ oriented along the [111] direction alters the shape of diffuse scattering in reciprocal space, but does not eliminate the scattering as would be expected in the case of a classic ferroelectric material. This suggests that a field-induced redistribution of the PNR has taken place.
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Local inhomogeneities known as polar nanoregions (PNR) play a key role in governing the dielectric properties of relaxor ferroelectrics - a special class of material that exhibits an enormous electromechanical response and is easily polarized with an external field. Using neutron inelastic scattering methods, we show that the PNR can also significantly affect the structural properties of the relaxor ferroelectric Pb(Zn1/3Nb2/3)O3-4.5%PbTiO3 (PZN-4.5%PT). A strong interaction is found between the PNR and the propagation of sound waves, i.e. acoustic phonons, the visibility of which can be enhanced with an external electric field. A comparison between acoustic phonons propagating along different directions reveals a large asymmetry in the lattice dynamics that is induced by the PNR. We suggest that a phase instability induced by this PNR-phonon interaction may contribute to the ultrahigh piezoelectric response of this and related relaxor ferroelectric materials. Our results also naturally explain the emergence of the various observed monoclinic phases in these systems.
We report neutron inelastic scattering experiments on single crystal PbMg$_{1/3}$Nb$_{2/3}$O$_{3}$ doped with 32% PbTiO$_{3}$, a relaxor ferroelectric that lies close to the morphotropic phase boundary. When cooled under an electric field $mathbf{E} parallel$ [001] into tetragonal and monoclinic phases, the scattering cross section from transverse acoustic (TA) phonons polarized parallel to $mathbf{E}$ weakens and shifts to higher energy relative to that under zero-field-cooled conditions. Likewise, the scattering cross section from transverse optic (TO) phonons polarized parallel to $mathbf{E}$ weakens for energy transfers $4 leq hbar omega leq 9$ meV. However, TA and TO phonons polarized perpendicular to $mathbf{E}$ show no change. This anisotropic field response is similar to that of the diffuse scattering cross section, which, as previously reported, is suppressed when polarized parallel to $mathbf{E}$, but not when polarized perpendicular to $mathbf{E}$. Our findings suggest that the lattice dynamics and dynamic short-range polar correlations that give rise to the diffuse scattering are coupled.
The response of polar nanoregions (PNR) in the relaxor compound Pb[(Zn$_{1/3}$Nb$_{2/3}$)$_{0.92}$Ti$_{0.08}$]O$_3$ subject to a [111]-oriented electric field has been studied by neutron diffuse scattering. Contrary to classical expectations, the diffuse scattering associated with the PNR persists, and is even partially enhanced by field cooling. The effect of the external electric field is retained by the PNR after the field is removed. The ``memory of the applied field reappears even after heating the system above $T_C$, and cooling in zero field.
We report measurements of the neutron diffuse scattering in a single crystal of the relaxor ferroelectric material 95.5%Pb(Zn1/3Nb2/3)O3-4.5%PbTiO3 (PZN-4.5%PT). We show that the diffuse scattering at high temperatures has a quasielastic component with energy width $agt$ 0.1 meV. On cooling the total diffuse scattering intensity increases, but the intensity and the energy width of the quasielastic component gradually diminish. At 50 K the diffuse scattering is completely static (i.e.the energy width lies within the limits of our instrumental resolution). This suggests that the dynamics of the short-range correlated atomic displacements associated with the diffuse scattering freeze at low temperature. We find that this depends on the wave vector q as the quasielastic diffuse scattering intensities associated with <001> (T1-type) and <110> (T2-type) atomic displacements vary differently with temperature and electric field.
(TMTTF)2AsF6 undergoes two phase transitions upon cooling from 300 K. At Tco=103 K a charge-ordering (CO) occurs, and at Tsp(B=9 T)=11 K the material undergoes a spin-Peierls (SP) transition. Within the intermediate, CO phase, the charge disproportionation ratio is found to be at least 3:1 from carbon-13 NMR 1/T1 measurements on spin-labeled samples. Above Tsp, up to about 3Tsp, 1/T1 is independent of temperature, indicative of low-dimensional magnetic correlations. With the application of about 0.15 GPa pressure, Tsp increases substantially, while Tco is rapidly suppressed, demonstrating that the two orders are competing. The experiments are compared to results obtained from calculations on the 1D extended Peierls-Hubbard model.
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