arXiv subjects

P. M. Gehring

Publications and source records attributed to P. M. Gehring.

At least 37 records · Page 2Linked to original sources

arXiv2010

Single Crystal Study of Competing Rhombohedral and Monoclinic Order in Lead Zirconate Titanate

Neutron diffraction data obtained on single crystals of PbZr1-xTixO3 with x = 0.325 and x = 0.460, which lie on the pseudorhombohedral side of the morphotropic phase boundary, suggest a coexistence of rhombohedral (R3m/R3c) and monoclinic (Cm) domains and that monoclinic order is enhanced by Ti substitution. A monoclinic phase with a doubled unit cell (Cc) is ruled out as the ground state.

cond-mat.mtrl-sci↗

arXiv2010

A two-component model of the neutron diffuse scattering in the relaxor ferroelectric PZN-4.5%PT

We report measurements of the neutron diffuse scattering in a single crystal of the relaxor ferroelectric material 95.5%Pb(Zn$_{1/3}$Nb$_{2/3}$)O$_3$-4.5%PbTiO$_3$ (PZN-4.5%PT). Our results suggest that the nanometer scale structure in this compound exhibits both $<100>$ and $<110>$ polarizations, which contribute to different portions of the total diffuse scattering intensity. These contributions can be distinguished by the differing responses to an electric field applied along [001]. While diffuse scattering intensities associated with $<110>$ (T2-type) polarizations show little to no change in a [001] field, those associated with $<100>$ (T1-type) polarizations are partially suppressed by the field at temperatures below the Curie temperature \emph{T$_C$} $\sim 475$ K. Neutron spin-echo measurements show that the diffuse scattering at (0.05,0,1) is largely dynamic at high temperature and gradually freezes on cooling, becoming mostly static at 200 K.

cond-mat.mtrl-sci↗

arXiv2010

Interplay between static and dynamic polar correlations in relaxor Pb(Mg_{1/3}Nb_{2/3})O_{3}

We have characterized the dynamics of the polar nanoregions in Pb(Mg$_{1/3}$Nb$_{2/3}$)O$_{3}$ (PMN) through high-resolution neutron backscattering and spin-echo measurements of the diffuse scattering cross section. We find that the diffuse scattering intensity consists of \emph{both} static and dynamic components. The static component first appears at the Curie temperature $Θ\sim 400$ K, while the dynamic component freezes completely at the temperature T$_{f} \sim 200$ 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 timescale of $\sim 1$ ns. Our neutron scattering results can thus be directly related to dielectric and infra-red 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.

cond-mat.mtrl-sci↗

arXiv2009

Soft phonon columns on the edge of the Brillouin zone in the relaxor PbMg1/3Nb2/3O3

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: \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.

cond-mat.mtrl-sci↗

arXiv2009

A reassessment of the Burns temperature and its relationship to the diffuse scattering, lattice dynamics, and thermal expansion in the relaxor PMN

We have used neutron scattering techniques to characterize the diffuse scattering and lattice dynamics in single crystals of the relaxor PMN from 10K to 900K. We observed two distinct types of diffuse scattering. The first is weak, relatively temperature independent, persists to at least 900 K, and forms bow-tie-shaped patterns in reciprocal space centered on (h00) Bragg peaks. We associate this primarily with chemical short-range order. The second is strong, temperature dependent, and forms butterfly-shaped patterns centered on (h00) Bragg peaks. This diffuse scattering has been attributed to the PNR because it responds to an electric field and vanishes near Td ~ 620K when measured with thermal neutrons. Surprisingly, it vanishes at 420K when measured with cold neutrons, which provide ~4 times superior energy resolution. That this onset temperature depends on the instrumental energy resolution demands a reassessment of the Burns temperature Td. Neutron backscattering measurements made with 300 times better energy resolution confirm the onset temperature of 420+/-20K. The energy width of the diffuse scattering is resolution limited, indicating that the PNR are static on timescales of at least 2 nsec. Transverse acoustic (TA) phonon lifetimes are temperature independent up to 900K for q < 0.2 1/A. This motivates a physical picture in which sufficiently long-wavelength TA phonons average over the PNR; only those TA phonons having wavelengths comparable to the size of the PNR are affected. The PMN lattice constant changes by less than 0.001 Angstroms below 300K, but expands rapidly at a rate of 2.5x10^-5 1/K at high temperature. The regimes of low and high thermal expansion bracket the revised value of Td, which suggests the anomalous thermal expansion results from the condensation of static PNR.

cond-mat.mtrl-sci↗

arXiv2008

The effect of local dipole moments on the structure and lattice dynamics of K0.98Li0.02TaO3

We present high energy x-ray (67 keV) and neutron scattering measurements on a single crystal of K$_{1-x}$Li$_x$TaO$_3$ for which the Li content ($x=0.02$) is less than $x_c = 0.022$, the critical value below which no structural phase transitions have been reported in zero field. While the crystal lattice does remain cubic down to T=10 K under both zero-field and field-cooled ($E \le 4$ kV/cm) conditions, indications of crystal symmetry lowering are seen at $T_C=63$ K where the Bragg peak intensity changes significantly. A strong and frequency-dependent dielectric permittivity is observed at ambient pressure, a defining characteristic of relaxors. However an extensive search for static polar nanoregions, which is also widely associated with relaxor materials, detected no evidence of elastic neutron diffuse scattering between 300 K and 10 K. Neutron inelastic scattering methods were used to characterize the transverse acoustic and optic phonons (TA1 and TO1 modes) near the (200) and (002) Bragg peaks. The zone center TO1 mode softens monotonically with cooling but never reaches zero energy in either zero field or in external electric fields of up to 4 kV/cm. These results are consistent with the behavior expected for a dipolar glass in which the local polar moments are frozen and exhibit no long-range order at low temperatures.

cond-mat.mtrl-sci↗

arXiv2008

Response of polar nanoregions in 68%Pb(Mg1/3Nb2/3)O3-32%PbTiO3 to a [001] electric field

We report neutron diffuse scattering measurements on a single crystal of 68%Pb(Mg1/3Nb2/3)O3-32%PbTiO3. Strong diffuse scattering is observed at low temperatures. An external field applied along the [001] direction affects the diffuse scattering in the (HK0) plane significantly, suggesting a redistribution occurs between polar nanoregions of different polarizations perpendicular to the field. By contrast, the [001] field has no effect on the diffuse scattering in the (HOL) and (0KL) zones.

cond-mat.mtrl-sci↗

arXiv2008

Phase instability induced by polar nanoregions in a relaxor ferroelectric system

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.

cond-mat.mtrl-sci↗

arXiv2007

Neutron and X-ray diffraction study of cubic [111] field cooled Pb(Mg1/3Nb2/3)O3

Neutron and x-ray diffraction techniques have been used to study the competing long and short-range polar order in the relaxor ferroelectric Pb(Mg$_{1/3}$Nb$_{2/3}$)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$^{\circ}$-$α$ =0.03$^{\circ}$)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$^{\circ}$-$α$=0.08 $\pm$ 0.03$^{\circ}$ 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 lineshape 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 maybe necessary for a relaxor ground state.

cond-mat.mtrl-sci↗

arXiv2006

The Anomalous Skin Effect in Single Crystal Relaxor Ferroelectric PZN-xPT and PMN-xPT

X-ray and neutron scattering studies of the lead-based family of perovskite relaxors PZN-$x$PT and PMN-$x$PT have documented a highly unusual situation in which the near-surface region of a single crystal can exhibit a structure that is different from that of the bulk when cooled to low temperatures. The near-surface region, or "skin" can also display critical behavior that is absent in the crystal interior, as well as a significantly different lattice spacing. By varying the incident photon energy, and thus the effective penetration depth, x-ray measurements indicate a skin thickness of order 10 $μ$m to 50 $μ$m for PZN-$x$PT samples with $0 \le x \le 8$%. Neutron residual stress measurements on a large PMN single crystal reveal a uniform lattice spacing within the bulk, but an increased strain near the surface. The presence of this skin effect has led to incorrect phase diagrams for both the PZN-$x$PT and PMN-$x$PT systems and erroneous characterizations of the nature of the relaxor state.

cond-mat.mtrl-sci↗

arXiv2006

Coexistence and competition of local- and long-range polar orders in a ferroelectric relaxor

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.

cond-mat.mtrl-sci↗

arXiv2005

The Persistence and Memory of Polar Nano-Regions in a Ferroelectric Relaxor Under an Electric Field

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.

cond-mat.mtrl-sci↗

arXiv2004

Cold neutron scattering study on diffuse and phonon excitations in the relaxor PbMg(1/3)Nb(2/3)O3

Cold neutron scattering experiments have been performed to explore the energy, temperature, and wave-vector dependence of the diffuse scattering and the transverse acoustic (TA) phonons in the relaxor PbMg(1/3)Nb(2/3)O3. We have observed a weak, but definitive, diffuse scattering cross section above the Burns temperature T_d ~ 600 K. This cross section, which is most likely caused by chemical short-range order, persists down to 100 K, and coexists with the much stronger diffuse scattering that is attributed to the polar nanoregions. A systematic study of the TA phonon around (1, 1, 0) has also been carried out. The phonon is well defined for small wave vectors q, but broadens markedly around q = (0.1, -0.1, 0).

cond-mat.mtrl-sci↗

arXiv2004

Interplay of structural and electronic phase separation in single crystalline La(2)CuO(4.05) studied by neutron and Raman scattering

We report a neutron and Raman scattering study of a single-crystal of La(2)CuO(4.05) prepared by high temperature electrochemical oxidation. Elastic neutron scattering measurements show the presence of two phases, corresponding to the two edges of the first miscibility gap, all the way up to 300 K. An additional oxygen redistribution, driven by electronic energies, is identified at 250 K in Raman scattering (RS) experiments by the simultaneous onset of two-phonon and two-magnon scattering, which are fingerprints of the insulating phase. Elastic neutron scattering measurements show directly an antiferromagnetic ordering below a Néel temperature of T_N =210K. The opening of the superconducting gap manifests itself as a redistribution of electronic Raman scattering below the superconducting transition temperature, T_c = 24K. A pronounced temperature-dependent suppression of the intensity of the (100) magnetic Bragg peak has been detected below T_c. We ascribe this phenomenon to a change of relative volume fraction of superconducting and antiferromagnetic phases with decreasing temperature caused by a form of a superconducting proximity effect.

cond-mat.supr-con↗

arXiv2004

X-ray and Neutron Diffraction Investigations of the Structural Phase Transformation Sequence under Electric Field in 0.7Pb(Mg1/3Nb2/3)-0.3PbTiO3 Crystals

The structural phase transformations of 0.7Pb(Mg1/3Nb2/3)O3-0.3PbTiO3 (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 (or ZFC) condition; (ii) C->T-> monoclinic (MC)-> monoclinic (MA) in the field-cooled (or FC) condition; and (iii) R->MA->MC->T with increasing field at fixed temperature beginning from the ZFC condition. Upon removal of the field, the MA 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 MA phase; (ii) a difference in lattice parameters between inside bulk and outside layer regions; and (iii) the diffuse nature of the MA and MC phase transition.

cond-mat.mtrl-sci↗

arXiv2004

High q-resolution neutron scattering technique using triple-axis spectrometers

We present a new technique which brings a substantial increase of the wave-vector $q$-resolution of triple-axis-spectrometers by matching the measurement wave-vector $q$ to the reflection $τ_a$ of a perfect crystal analyzer. A relative Bragg width of $δ/Q \sim 10^{-4}$ can be achieved with reasonable collimation settings. This technique is very useful in measuring small structural changes and line broadenings that can not be accurately measured with conventional set-ups, while still keeping all the strengths of a triple-axis-spectrometer.

cond-mat.other↗

arXiv2003

Evidence of decoupled lattice distortion and ferroelectric polarization in the relaxor system PMN-xPT

We report high $q$-resolution neutron scattering data on PMN-$x$PT 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$_C \sim 375$ K. Our data provide conclusive evidence that a new 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.

cond-mat.mtrl-sci↗

arXiv2003

A Neutron Elastic Diffuse Scattering Study of PMN

We have performed elastic diffuse neutron scattering studies on the relaxor Pb(Mg$_{1/3}$Nb$_{2/3}$)O$_3$ (PMN). The measured intensity distribution near a (100) Bragg peak in the (hk0) scattering plane assumes the shape of a butterfly with extended intensity in the (110) and (1$\bar{1}$0) directions. The temperature dependence of the diffuse scattering shows that both the size of the polar nanoregions (PNR) and the integrated diffuse intensity increase with cooling even for temperatures below the Curie temperature $T_C \sim 213$ K.

cond-mat.mtrl-sci↗