Browsing by Author "Gehring, Peter M."
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- Dynamic origin of the morphotropic phase boundary: Soft modes and phase instability in 0.68Pb(Mg(1/3)Nb(2/3)O(3))-0.32PbTiO(3)Cao, Hu; Stock, Chris; Xu, Guangyong; Gehring, Peter M.; Li, Jiefang; Viehland, Dwight D. (American Physical Society, 2008-09-04)We report neutron inelastic scattering and high-resolution x-ray diffraction measurements on single crystal 0.68Pb(Mg(1/3)Nb(2/3)O(3))-0.32PbTiO(3)) (PMN-0.32PT), a relaxor ferroelectric material that lies within the compositional range of the morphotropic phase boundary (MPB) where the piezoelectric properties of PMN-xPT compounds are close to maximal. Data were obtained between 100 and 600 K under zero and nonzero electric field applied along the cubic [001] direction. The lowest-energy, zone-center, transverse optic phonon is strongly damped and softens slowly at high temperature; however, the square of the soft-mode energy begins to increase linearly with temperature as in a conventional ferroelectric, which we term the soft-mode "recovery," upon cooling into the tetragonal phase at T(C). Our data show that the soft mode in PMN-0.32PT behaves almost identically to that in pure PMN, exhibiting the same temperature dependence and recovery temperature even though PMN exhibits no well-defined structural transition (no T(C)). The temperature dependence of the soft mode in PMN-0.32PT is also similar to that in PMN-0.60PT; however, in PMN-0.60PT the recovery temperature equals T(C). These results suggest that the temperature dependence and the energy scale of the soft-mode dynamics in PMN-xPT are independent of concentration on the Ti-poor side of the MPB, but scale with T(C) for Ti-rich compositions. Thus the MPB may be defined in lattice dynamical terms as the concentration where T(C) first matches the recovery temperature of the soft mode. High-resolution x-ray studies show that the cubic-to-ferroelectric phase boundary shifts to higher temperatures by an abnormal amount within the MPB region in the presence of an electric field. This suggests that an unusual instability exists within the apparently cubic phase at the MPB.
- Evidence for anisotropic polar nanoregions in relaxor Pb(Mg1/3Nb2/3)O-3: A neutron study of the elastic constants and anomalous TA phonon damping in PMNStock, Chris; Gehring, Peter M.; Hiraka, Haruhiro; Swainson, I. P.; Xu, Guangyong; Ye, Z. G.; Luo, Hongjie; Li, Jiefang; Viehland, Dwight D. (American Physical Society, 2012-09-18)We use neutron inelastic scattering to characterize the acoustic phonons in the relaxor Pb(Mg1/3Nb2/3)O-3 (PMN) and demonstrate the presence of a highly anisotropic damping mechanism that is directly related to short-range polar correlations. For a large range of temperatures above T-c similar to 210 K, where dynamic, short-range polar correlations are present, acoustic phonons propagating along [1 (1) over bar0] and polarized along [110] (TA(2) phonons) are overdamped and softened across most of the Brillouin zone. By contrast, acoustic phonons propagating along [100] and polarized along [001] (TA(1) phonons) are overdamped and softened for a more limited range of wave vectors q. The anisotropy and temperature dependence of the acoustic phonon energy linewidth Gamma are directly correlated with neutron diffuse scattering cross section, indicating that polar nanoregions are the cause of the anomalous behavior. The damping and softening vanish for q -> 0, i.e., for long-wavelength acoustic phonons near the zone center, which supports the notion that the anomalous damping is a result of the coupling between the relaxational component of the diffuse scattering and the harmonic TA phonons. Therefore, these effects are not due to large changes in the elastic constants with temperature because the elastic constants correspond to the long-wavelength limit. We compare the elastic constants we measure to those from Brillouin scattering experiments and to values reported for pure PbTiO3. We show that while the values of C-44 are quite similar, those for C-11 and C-12 are significantly less in PMN and result in a softening of (C-11 - C-12) over PbTiO3. The elastic constants also show an increased elastic anisotropy [2C(44)/(C-11 - C-12)] in PMN versus that in PbTiO3. These results are suggestive of an instability to TA(2) acoustic fluctuations in PMN and other relaxor ferroelectrics. We discuss our results in the context of the current debate over the "waterfall" effect and show that they are inconsistent with acoustic-optic phonon coupling or other models that invoke the presence of a second, low-energy optic mode.
- Evidence of decoupled lattice distortion and ferroelectric polarization in the relaxor system PMN-xPTXu, Guangyong; Viehland, Dwight D.; Li, Jiefang; Gehring, Peter M.; Shirane, Gen (American Physical Society, 2003-12-30)We report high q-resolution neutron scattering data on PMN-xPT single crystals with x=20% and 27%. No rhombohedral distortion occurs in the 20PT sample for temperatures as low as 50 K. On the other hand, the 27PT sample transforms into a rhombohedral phase below T(C)similar to375 K. Our data provide conclusive evidence that a phase with an average cubic lattice is present in the bulk of this relaxor system at low PT concentration, in which the ferroelectric polarization and lattice distortion are decoupled. The rhombohedral distortion is limited to the outermost tens of microns of the crystal.
- Interplay between static and dynamic polar correlations in relaxor Pb(Mg1/3Nb2/3)O-3Stock, Chris; Van Eijck, L.; Fouquet, P.; Maccarini, M.; Gehring, Peter M.; Xu, Guangyong; Luo, Hongjie; Zhao, X.; Li, Jiefang; Viehland, Dwight D. (American Physical Society, 2010-04-01)We have characterized the dynamics of the polar nanoregions in Pb(Mg1/3Nb2/3)O-3 through high-resolution neutron-backscattering and spin-echo measurements of the diffuse-scattering cross section. We find that the diffuse-scattering intensity consists of both static and dynamic components. The static component first appears at the Curie temperature Theta similar to 400 K while the dynamic component freezes completely at the temperature T-f similar to 200 K; together, these components account for all of the observed spectral weight contributing to the diffuse-scattering cross section. The integrated intensity of the dynamic component peaks near the temperature at which the frequency-dependent dielectric constant reaches a maximum (T-max) when measured at 1 GHz, i.e., on a time scale of similar to 1 ns. Our neutron-scattering results can thus be directly related to dielectric and infrared measurements of the polar nanoregions. Finally, the global temperature dependence of the diffuse scattering can be understood in terms of just two temperature scales, which is consistent with random-field models.
- Lead-free and lead-based ABO(3) perovskite relaxors with mixed-valence A-site and B-site disorder: comparative neutron scattering structural study of (Na1/2Bi1/2) TiO3 and Pb(Mg1/3Nb2/3)O-3Ge, Wenwei; Devreugd, Christopher P.; Phelan, Daniel; Zhang, Qinhui; Ahart, Muhtar; Li, Jiefang; Luo, Haosu; Boatner, Lynn A.; Viehland, Dwight D.; Gehring, Peter M. (American Physical Society, 2013-11-01)We report the results of neutron elastic-scattering measurements made between -250 degrees C and 620 degrees C on the lead-free relaxor (Na1/2Bi1/2)TiO3 (NBT). Strong, anisotropic, elastic diffuse scattering intensity decorates the (100), (110), (111), (200), (210), and (220) Bragg peaks at room temperature. The wave-vector dependence of this diffuse scattering is compared to that in the lead-based relaxor Pb(Mg1/3Nb2/3)O-3 (PMN) to determine if any features might be common to relaxors. Prominent ridges in the elastic diffuse scattering intensity contours that extend along < 110 > are seen that exhibit the same zone dependence as those observed in PMN and other lead-based relaxors. These ridges disappear gradually on heating above the cubic-to-tetragonal phase transition temperature T-CT = 523 degrees C, which is also near the temperature at which the dielectric permittivity begins to deviate from Curie-Weiss behavior. We thus identify the < 110 >-oriented ridges as a relaxor-specific property. The diffuse scattering contours also display narrower ridges oriented along < 100 > that are consistent with the x-ray results of Kreisel et al. [Phys. Rev. B 68, 014113 (2003)]; these vanish near 320 degrees C, indicating that they have a different physical origin. The < 100 >-oriented ridges are not observed in PMN. We observe no equivalent relaxor-specific elastic diffuse scattering from the homovalent relaxor analogues K0.95Li0.05TiO3 (A-site disordered) and KTa0.95Nb0.05O3 (B-site disordered). This suggests that the < 110 >-oriented diffuse scattering ridges are correlated with the presence of strong random electric fields and invites a reassessment of what defines the relaxor phase. We find that doping NBT with 5.6% BaTiO3, a composition close to the morphotropic phase boundary with enhanced piezoelectric properties, increases the room-temperature correlation length along [1 (1) over bar0] from 40 to 60 angstrom while doubling the associated integrated diffuse scattering. Similar behavior was reported by Matsuura et al. [Phys. Rev. B 74, 144107 (2006)] for morphotropic compositions of PMN doped with PbTiO3. Finally, we comment on the recent observation of monoclinicity in NBT at room temperature by placing a strict bound on the strength of the (1/2 1/2 1/2) superlattice reflection associated with the Cc space group based on the atomic coordinates published in the x-ray study by Aksel et al. [Appl. Phys. Lett. 98, 152901 (2011)] for NBT. We show that a skin effect, analogous to that reported in the relaxors PZN-xPT and PMN-xPT, can reconcile our neutron single-crystal data with the x-ray powder data of Aksel et al. [Appl. Phys. Lett. 98, 152901 (2011)]. Our finding of a skin effect in a lead-free, A-site disordered, heterovalent relaxor supports the idea that it arises in the presence of strong random electric fields.
- Neutron and x-ray diffraction study of cubic [111] field-cooled Pb(Mg1/3Nb2/3)O-3Stock, Chris; Xu, Guangyong; Gehring, Peter M.; Luo, Hongjie; Zhao, X.; Cao, Hu; Li, Jiefang; Viehland, Dwight D.; Shirane, Gen (American Physical Society, 2007-08-01)Neutron and x-ray diffraction techniques have been used to study the competing long- and short-range polar order in the relaxor ferroelectric Pb(Mg1/3Nb2/3)O-3 (PMN) under a [111] applied electric field. Despite reports of a structural transition from a cubic phase to a rhombohedral phase for fields E>1.7 kV/cm, we find that the bulk unit cell remains cubic (within a sensitivity of 90 degrees-alpha=0.03 degrees) for fields up to 8 kV/cm. Furthermore, we observe a structural transition confined to the near surface volume or "skin" of the crystal where the cubic cell is transformed to a rhombohedral unit cell at T-c=210 K for E>4 kV/cm, for which 90 degrees-alpha=0.08 +/- 0.03 degrees below 50 K. While the bulk unit cell remains cubic, a suppression of the diffuse scattering and concomitant enhancement of the Bragg peak intensity is observed below T-c=210 K, indicating a more ordered structure with increasing electric field yet an absence of a long-range ferroelectric ground state in the bulk. The electric field strength has little effect on the diffuse scattering above T-c, however, below T-c the diffuse scattering is reduced in intensity and adopts an asymmetric line shape in reciprocal space. The absence of hysteresis in our neutron measurements (on the bulk) and the presence of two distinct temperature scales suggests that the ground state of PMN is not a frozen glassy phase as suggested by some theories but is better understood in terms of random fields introduced through the presence of structural disorder. Based on these results, we also suggest that PMN represents an extreme example of the two-length scale problem, and that the presence of a distinct skin may be necessary for a relaxor ground state.
- Role of Nanoscale Precipitates on the Enhanced Magnetostriction of Heat-Treated Galfenol (Fe1-xGax) AlloysCao, Hu; Gehring, Peter M.; Devreugd, Christopher P.; Rodriguez-Rivera, J. A.; Li, J.; Viehland, Dwight D. (American Physical Society, 2009-03-27)We report neutron diffuse scattering measurements on highly magnetostrictive Fe1-xGax alloys (0.14 < x < 0.20) with different thermal treatments. This diffuse scattering scales with magnetostriction and exhibits asymmetric peaks at the (100) and (300) reciprocal lattice positions that are consistent with the coexistence of short-range ordered, coherent nanometer-scale precipitates embedded in a long-range ordered, body-centered cubic matrix. A large peak splitting is observed at (300) for x=0.19, which indicates that the nanoprecipitates are not cubic and have a large elastic strain. This implies a structural origin for the enhanced magnetostriction.
- Soft phonon columns on the edge of the Brillouin zone in the relaxor PbMg1/3Nb2/3O3Swainson, I. P.; Stock, Chris; Gehring, Peter M.; Xu, Guangyong; Hirota, K.; Qiu, Y.; Luo, Hongjie; Zhao, X.; Li, Jiefang; Viehland, Dwight D. (American Physical Society, 2009-06-10)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. Unusual "columns" of phonon scattering that are localized in momentum, but extended in energy, are seen at both high-symmetry points along the zone edge: (Q) over right arrowR= {1/2,1/2,1/2} and (Q) over right arrowM={1/2,1/2,0}. These columns soften at similar to 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 Pb2+ and O2- 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.
- X-ray and neutron diffraction investigations of the structural phase transformation sequence under electric field in 0.7Pb(Mg1/3Nb2/3)-0.3PbTiO(3) crystalBai, Feiming; Wang, Naigang; Li, Jiefang; Viehland, Dwight D.; Gehring, Peter M.; Xu, Guangyong; Shirane, Gen (American Institute of Physics, 2004-08-01)The structural phase transformations of 0.7Pb(Mg1/3Nb2/3)O-3-0.3PbTiO(3) (PMN-30%PT) have been studied using x-ray diffraction (XRD) and neutron scattering as a function of temperature and electric field. We observe the phase transformational sequence (i) cubic (C)--> tetragonal (T)--> rhombohedral (R) in the zero-field-cooled (ZFC) condition; (ii) C-->T--> monoclinic (M-C)--> monoclinic (M-A) in the field-cooled (FC) condition; and (iii) R-->M-A-->M-C-->T with increasing field at fixed temperature beginning from the ZFC condition. Upon removal of the field, the M-A phase is stable at room temperature in the FC condition, and also in the ZFC condition with increasing field. Several subtleties of our findings are discussed based on results from thermal expansion and dielectric measurements, including (i) the stability of the M-A phase, (ii) a difference in lattice parameters between inside bulk and outside layer regions, and (iii) a difference in the phase transition temperature between XRD and dielectric data. (C) 2004 American Institute of Physics.
- X-ray diffraction study of the pressure-induced bcc-to-hcp phase transition in the highly magnetostrictive Fe0.81Ga0.19 alloyAhart, Muhtar; Devreugd, Christopher P.; Li, Jiefang; Viehland, Dwight D.; Gehring, Peter M.; Hemley, Russell J. (American Physical Society, 2013-11-07)High-pressure x-ray diffraction measurements were performed at room temperature on single crystals of the highly magnetostrictive alloy Fe0.81Ga0.19 (galfenol). This alloy has a bcc crystal structure at ambient pressure but undergoes a bcc-to-hcp phase transition at 24 GPa on compression. A large hysteresis loop is observed in which the reversed transition occurs at 13 GPa on decompression. The midpoint of this transition is 18.5 GPa. The measured bulk modulus of this material is 182 (+/- 17) GPa, which is comparable to that of pure iron. As with iron, the hcp structure of the alloy can be derived from a compression of the bcc lattice along [001] that is accompanied by shearing along [1 (1) over bar0]. Our results indicate that the addition of Ga shifts the bcc-to-hcp transition from 13 GPa in pure iron to 18.5 GPa, and we speculate that this is due to the larger atomic radius of Ga. A uniaxial loading of 3 GPa completely suppresses the diffuse scattering in Fe0.81Ga0.19. We ascertain that the magnetostrictive properties of the alloy are reduced under pressure.