arXiv subjects

C. Stock

Publications and source records attributed to C. Stock.

At least 109 records · Page 6Linked to original sources

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↗

arXiv2009

Magnetic field resonantly enhanced free spins in underdoped YBa$_{2}$Cu$_{3}$O$_{6+x}$

Using neutron scattering, we investigate the effect of a magnetic field on the static and dynamic spin response in heavily underdoped superconducting YBa$_{2}$Cu$_{3}$O$_{6+x}$ (YBCO$_{6+x}$) with x=0.33 (T$_{c}$=8 K) and 0.35 (T$_{c}$=18 K). In contrast to the heavily doped and superconducting monolayer cuprates, the elastic central peak characterizing static spin correlations does not respond observably to a magnetic field which suppresses superconductivity. Instead, we find a magnetic field induced resonant enhancement of the spin fluctuations. The energy scale of the enhanced fluctuations matches the Zeeman energy within both the normal and vortex phases while the momentum dependence is the same as the zero field bilayer response. The magnitude of the enhancement is very similar in both phases with a fractional intensity change of $(I/I_{0}-1) \sim 0.1$. We suggest that the enhancement is not directly correlated with superconductivity but is the result of almost free spins located near hole rich regions.

cond-mat.supr-con↗

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

Orbital ordering promotes weakly-interacting S=1/2 dimers in the triangular lattice compound Sr3Cr2O8

The weakly interacting S=1/2 dimers system Sr3Cr2O8 has been investigated by powder neutron diffraction and inelastic neutron scattering. Our data reveal a structural phase transition below room temperature corresponding to an antiferro-orbital ordering with nearly 90 degrees arrangement of the occupied 3z^2-r^2 d-orbital. This configuration leads to a drastic reduction of the inter-dimer exchange energies with respect to the high temperature orbital-disorder state, as shown by a spin-dimer analysis of the super-superexchange interactions performed using the Extended Huckel Tight Binding method. Inelastic neutron scattering reveals the presence of a quasi non-dispersive magnetic excitation at 5.4 meV, in agreement with the picture of weakly-interacting dimers.

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↗

arXiv2008

Spin dynamics near the critical doping in weakly-superconducting underdoped YBa2Cu3O6.35 (Tc=18K)

Using neutron scattering we have determined the magnetic structure and fluctuations in the YBa2Cu3O6.35 superconductor (Tc=18 K). The long-range ordered collinear spins of the insulating antiferromagnet are replaced by a commensurate central mode arising from slow, isotropically polarized, short-range spin correlations. The inelastic spectrum up to 30 meV is broad in wave vector and commensurate. In contrast to the the resonance peak of higher Tc superconductors, the spins exhibit a single overdamped spectrum whose rate of relaxation decreases on cooling and saturates at 5 meV below 50 K. As the relaxation rate saturates the quasi-static spin correlations grow and become resolution limited in energy. The spin susceptibility at high temperatures illustrates that the dominant energy scale is set by the temperature. At low temperatures, the scale length is geometric and not linked by velocity to dynamic widths. There is no observable suppression of the spin fluctuations or central mode upon the onset of superconductivity. The spins respond not to coherent charge pairs but to hole doping allowing coexistence of glassy short range spin order with superconductivity. Since the physics of the weakly superconducting system YBCO6.35 must connect continuously with that in more strongly superconducting YBCO6.5, we find that neither incommensurate stripe-like spin modulations nor a well-defined neutron spin resonance are essential for the onset with doping of pairing in a high temperature cuprate superconductor.

cond-mat.supr-con↗

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↗

arXiv2007

Spin resonance in the d-wave superconductor CeCoIn5

Neutron scattering is used to probe antiferromagnetic spin fluctuations in the d-wave heavy fermion superconductor CeCoIn$_{5}$ (T$_{c}$=2.3 K). Superconductivity develops from a state with slow ($\hbarΓ$=0.3 $\pm$ 0.15 meV) commensurate (${\bf{Q_0}}$=(1/2,1/2,1/2)) antiferromagnetic spin fluctuations and nearly isotropic spin correlations. The characteristic wavevector in CeCoIn$_{5}$ is the same as CeIn$_{3}$ but differs from the incommensurate wavevector measured in antiferromagnetically ordered CeRhIn$_{5}$. A sharp spin resonance ($\hbarΓ<0.07$ meV) at $\hbar ω$ = 0.60 $\pm$ 0.03 meV develops in the superconducting state removing spectral weight from low-energy transfers. The presence of a resonance peak is indicative of strong coupling between f-electron magnetism and superconductivity and consistent with a d-wave gap order parameter satisfying $Δ({\bf q+Q_0})=-Δ({\bf q})$.

cond-mat.supr-con↗

arXiv2007

Evidence for decay of spin-waves above the pseudogap in underdoped YBa2Cu3O6.35

The magnetic spectrum at high-energies in heavily underdoped YBa$_{2}$Cu$_{3}$O$_{6.35}$ (T$_{c}$=18 K) has been determined throughout the Brillouin zone. At low-energy the scattering forms a cone of spin excitations emanating from the antiferromagnetic (0.5, 0.5) wave vector with an acoustic velocity similar to that of insulating cuprates. At high energy transfers, below the maximum energy of 270 meV at (0.5, 0), we observe zone boundary dispersion much larger and spectral weight loss more extensive than in insulating antiferromagnets. Moreover we report phenomena not found in insulators, an overall lowering of the zone-boundary energies and a large damping of $\sim$ 100 meV of the spin excitations at high-energies. The energy above which the damping occurs coincides approximately with the gap determined from transport measurements. We propose that as the energy is raised the spin excitations encounter an extra channel of decay into particle-hole pairs of a continuum that we associate with the pseudogap.

cond-mat.supr-con↗

arXiv2007

Quantum phase transitions in magnetism and superconductivity: emergent spin topology seen with neutrons

Magnetic spins and charges interact strongly in high-temperature superconductors. New physics emerges as layers of copper oxide are tuned towards the boundary of the superconducting phase. As the pseudogap increases the characteristic spin excitation energy decreases. We show that our well-annealed YBa2Cu3O6+x (YBCO6+x) single crystals are orthorhombic and superconducting but not antiferromagnetically ordered. Near the critical concentration for superconductivity for x = 0.35 the spins fluctuate on two energy scales, one a relaxational spin response at ~2 meV and the other a slow central mode that is resolution-limited in energy (<0.08 meV) but broad in momentum. The gradual formation on cooling of a central mode over a range of momenta suggests that the spin ground state from which coherent superconducting pairing emerges may be quantum disordered. We show that YBCO6.35 adopts a homogeneous state that consists of highly-organized frozen sub-critical three-dimensional spin correlations. The continuous spin evolution indicates that a single quantum state occurs in contrast to claims from site-based probes that lightly doped YBCO undergoes a transition to antiferromagnetic Bragg order followed by a sharp transition to a cluster glass phase. For x = 0.35, where Tc = 18 K is reduced to 1/5 of Tcmax, the spin ground state is reached without a sharp transition and consists of short correlations extending over only 8 Angstrom between cells and 42 Angstrom within the planes. Polarized neutrons show the angular spin distribution to be isotropic unlike the AF insulator. Since moment is conserved we interpret this as evidence for hole-induced spin rotations rather than decay.

cond-mat.supr-con↗

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

Magnetic neutron scattering in hole doped cuprate superconductors

A review is presented of the static and dynamic magnetic properties of hole-doped cuprate superconductors measured with neutron scattering. A wide variety of experiments are described with emphasis on the monolayer La_{2-x}(Sr,Ba)_{x}CuO_{4} and bilayer YBa_{2}Cu_{3}O_{6+x} cuprates. At zero hole doping, both classes of materials are antiferromagnetic insulators with large superexchange constants of J > 100 meV. For increasing hole doping, the cuprates become superconducting at a critical hole concentration of x_{c}=0.055. The development of new instrumentation at neutron beam sources coupled with the improvement in materials has lead to a better understanding of these materials and the underlying spin dynamics over a broad range of hole dopings. We will describe how the spin dispersion changes across the insulating to superconducting boundary as well as the static magnetic properties which are directly coupled with the superconductivity. Experiments directly probing the competing magnetic and superconducting order parameters involving magnetic fields, impurity doping, and structural order will be examined. Correlations between superconductivity and magnetism will also be discussed.

cond-mat.supr-con↗

arXiv2006

Damped Soft Phonons and Diffuse Scattering in 40PMN-60PT

Using neutron elastic and inelastic scattering and high-energy x-ray diffraction, we present a comparison of 40% Pb(Mg$_{1/3}$Nb$_{2/3}$)O$_{3}$-60% PbTiO$_{3}$ (PMN-60PT) with pure Pb(Mg$_{1/3}$Nb$_{2/3}$)O$_{3}$ (PMN) and PbTiO$_{3}$ (PT). We measure the structural properties of PMN-60PT to be identical to pure PT, however, the lattice dynamics are exactly that previously found in relaxors PMN and PZN. PMN-60PT displays a well-defined macroscopic structural transition from a cubic to tetragonal unit cell at 550 K. The diffuse scattering is shown to be weak indicating that the structural distortion is long-range in PMN-60PT and short-range polar correlations (polar nanoregions) are not present. Even though polar nanoregions are absent, the soft optic mode is short-lived for wavevectors near the zone-centre. Therefore, PMN-60PT displays the same waterfall effect as prototypical relaxors PMN and PZN. We conclude that it is random fields resulting from the intrinsic chemical disorder which is the reason for the broad transverse optic mode observed in PMN and PMN-60PT near the zone centre and not due to the formation of short-ranged polar correlations. Through our comparison of PMN, PMN-60PT, and pure PT, we interpret the dynamic and static properties of the PMN-xPT system in terms of a random field model in which the cubic anisotropy term dominates with increasing doping of PbTiO$_{3}$.

cond-mat.mtrl-sci↗

arXiv2006

Central mode and spin confinement near the boundary of the superconducting phase in YBa2Cu3O6.353 (Tc=18 K)

We have mapped the neutron scattering spin spectrum at low-energies in YBa2Cu3O6.353 (Tc=18 K) where the doping ~0.06 is near the critical value (pc=0.055) for superconductivity. No coexistence with long range ordered antiferromagnetism is found. The spins fluctuate on two energy scales, one a damped spin response with a ~2 meV relaxation rate and the other a central mode with a relaxation rate that slows to less than 0.08 meV below Tc. The spectrum mirrors that of a soft mode driving a central mode. Extremely short correlation lengths, 42+-5 Angstrom in-plane and 8+-2 Angstrom along the c direction, and isotropic spin orientations for the central mode indicate that the correlations are subcritical with respect to any second order transition to Neel order. The dynamics follows a model where damped spin fluctuations are coupled to the slow fluctuations of regions with correlations shortened by the hole doping.

cond-mat.supr-con↗

arXiv2004

From incommensurate to dispersive spin-fluctuations: The high-energy inelastic spectrum in superconducting YBa2Cu3O6.5

We have investigated the spin fluctuations at energy transfers up to ~110 meV, well above the resonance energy (33 meV) in the YBa2Cu3O6.5 ortho-II superconductor using neutron time-of-flight and triple-axis techniques. The spectrum at high energies differs from the low-energy incommensurate modulations previously reported where the incommensurate wave vector is largely independent of energy. Well above the resonance the peak of the spin response lies at wave vectors that increase with energy. Within error the excitations at all energies above the resonance are best described by a ring around the (pi, pi) position. The isotropic wave-vector pattern differs from a recently reported square pattern in different but related systems. The spin spectral weight at high-energies is similar to that in the insulator but the characteristic velocity is ~40% lower. We introduce a method of extracting the acoustic and optic weights at all energies from time-of-flight data. We find that the optic spectral weight extends to surprisingly low-energies of ~25 meV, and infer that the bilayer spin correlations weaken with increase in hole doping. When the low-energy optic excitations are taken into account we measure the total integrated weight around (pi, pi), for energies below 120 meV, to agree with that expected from the insulator. As a qualitative guide, we compare spin-wave calculations for an ordered and a disordered stripe model and describe the inadequacy of this and other stripe models for the high-energy fluctuations.

cond-mat.supr-con↗

arXiv2004

Enhancement of magnetic order in the incommensurate phase of Mg-doped CuGeO$_{3}$

We present elastic neutron scattering results at high magnetic fields for Mg-doped CuGeO$_{3}$. For low magnesium concentrations, where a spin-Peierls phase is present, we find an enhancement of the long range antiferromagnetic order in the structural incommensurate phase induced by a high magnetic field. In the incommensurate phase, the Néel temperature increases with field leading to a gain in the magnetic Bragg peak intensity at low temperatures. We also find that the magnetic Bragg peaks remain commensurate even though the structure is incommensurate at high magnetic fields due to the formation of solitons. We interpret these results in terms of the solitons formed at high-magnetic fields effectively acting as doped impurities. Our results point to a strongly disordered ground state with the the antiferromagnetic order localized around impurity sites.

cond-mat.str-el↗