arXiv subjects

C. Stock

Publications and source records attributed to C. Stock.

At least 73 records · Page 4Linked to original sources

arXiv2015

Determination of spin and orbital magnetization in the ferromagnetic superconductor UCoGe

The magnetism in the ferromagnetic superconductor UCoGe has been studied using a combination of magnetic Compton scattering, bulk magnetization, X-ray magnetic circular dichroism and electronic structure calculations, in order to determine the spin and orbital moments. The experimentally observed total spin moment, $M_s$, was found to be -0.24 $\pm$ 0.05~$μ_B$ at 5~T. By comparison with the total moment of 0.16 $\pm$ 0.01~$μ_B$, the orbital moment, $M_l$, was determined to be 0.40 $\pm$ 0.05~$μ_B$. The U and Co spin moments were determined to be antiparallel. We find that the U 5\textit{f} electrons carry a spin moment of U$_s \approx$ -0.30~$μ_B$ and that there is a Co spin moment of Co$_s \approx$ 0.06~$μ_B$ induced via hybridization. The ratio U$_l/$U$_s$, of $-1.3 \pm 0.3$, shows the U moment to be itinerant. In order to ensure an accurate description of the properties of 5\textit{f} systems, and to provide a critical test of the theoretical approaches, it is clearly necessary to obtain experimental data for both the spin and orbital moments, rather than just the total magnetic moment. This can be achieved simply by measuring the spin moment with magnetic Compton scattering and comparing this to the total moment from bulk magnetization.

cond-mat.str-el↗

arXiv2015

From soft harmonic phonons to fast relaxational dynamics in CH$_{3}$NH$_{3}$PbBr$_{3}$

The lead-halide perovskites, including CH$_{3}$NH$_{3}$PbBr$_{3}$, are components in cost effective, highly efficient photovoltaics, where the interactions of the molecular cations with the inorganic framework are suggested to influence the electronic and ferroelectric properties. CH$_{3}$NH$_{3}$PbBr$_{3}$ undergoes a series of structural transitions associated with orientational order of the CH$_{3}$NH$_{3}$ (MA) molecular cation and tilting of the PbBr$_{3}$ host framework. We apply high-resolution neutron scattering to study the soft harmonic phonons associated with these transitions, and find a strong coupling between the PbBr$_{3}$ framework and the quasistatic CH$_{3}$NH$_{3}$ dynamics at low energy transfers. At higher energy transfers, we observe a PbBr$_{6}$ octahedra soft mode driving a transition at 150 K from bound molecular excitations at low temperatures to relatively fast relaxational excitations that extend up to $\sim$ 50-100 meV. We suggest that these temporally overdamped dynamics enables possible indirect band gap processes in these materials that are related to the enhanced photovoltaic properties.

cond-mat.mtrl-sci↗

arXiv2015

Phonon coupling to dynamic short-range polar order in a relaxor ferroelectric near the morphotropic phase boundary

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 $4 \leq \hbar ω\leq 9$ 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.

cond-mat.mtrl-sci↗

arXiv2015

Unstable Spin-Ice Order in the Stuffed Metallic Pyrochlore Pr$_{2+x}$Ir$_{2-x}$O$_{7-δ}$

Specific heat, elastic neutron scattering, and muon spin rotation ($μ$SR) experiments have been carried out on a well-characterized sample of "stuffed" (Pr-rich) Pr$_{2+x}$Ir$_{2-x}$O$_{7-δ}$. Elastic neutron scattering shows the onset of long-range spin-ice "2-in/2-out" magnetic order at $T_M = 0.93$ K, with an ordered moment of 1.7(1)$μ_\mathrm{B}$/Pr ion at low temperatures. Approximate lower bounds on the correlation length and correlation time in the ordered state are 170 Å and 0.7 ns, respectively. $μ$SR experiments yield an upper bound 2.6(7) mT on the local field $B_\mathrm{loc}^{4f}$ at the muon site, which is nearly two orders of magnitude smaller than the expected dipolar field for long-range spin-ice ordering of 1.7$μ_B$ moments (120--270 mT, depending on muon site). This shortfall is due in part to splitting of the non-Kramers crystal-field ground-state doublets of near-neighbor Pr$^{3+}$ ions by the $μ^+$-induced lattice distortion. For this to be the only effect, however, $\sim$160 Pr moments out to a distance of $\sim$14 Å must be suppressed. An alternative scenario, which is consistent with the observed reduced nuclear hyperfine Schottky anomaly in the specific heat, invokes slow correlated Pr-moment fluctuations in the ordered state that average $B_\mathrm{loc}^{4f}$ on the $μ$SR time scale (${\sim}10^{-7}$ s), but are static on the time scale of the elastic neutron scattering experiments (${\sim}10^{-9}$ s). In this picture the dynamic muon relaxation suggests a Pr$^{3+}$ $4f$ correlation time of a few nanoseconds, which should be observable in a neutron spin echo experiment.

cond-mat.str-el↗

arXiv2015

Fluctuating defects in the incipient relaxor K$_{1-x}$Li$_x$TaO$_3$ (x=0.02)

We report neutron scattering measurements of the structural correlations associated with the apparent relaxor transition in K$_{1-x}$Li$_x$TaO$_3$ for $x=0.02$ (KLT(0.02)). This compound displays a broad and frequency-dependent peak in the dielectric permittivity, which is the accepted hallmark of all relaxors. However, no evidence of elastic diffuse scattering or any soft mode anomaly is observed in KLT(0.02) [J. Wen et al., Phys. Rev. B 78, 144202 (2008)], a situation that diverges from that in other relaxors such as PbMg$_{1/3}$Nb$_{2/3}$O$_3$. We resolve this dichotomy by showing that the structural correlations associated with the transition in KLT(0.02) are purely dynamic at all temperatures, having a timescale on the order of $\sim$THz. These fluctuations are overdamped, non-propagating, and spatially uncorrelated. Identical measurements made on pure KTaO$_3$ show that they are absent (within experimental error) in the undoped parent material. They exhibit a temperature dependence that correlates well with the dielectric response, which suggests that they are associated with local ferroelectric regions induced by the Li$^+$ doping. The ferroelectric transition that is induced by the introduction of Li$^+$ cations is therefore characterized by quasistatic fluctuations, which represents a stark contrast to the soft harmonic-mode-driven transition observed in conventional perovskite ferroelectrics like PbTiO$_3$. The dynamic, glass-like, structural correlations in KLT(0.02) are much faster than those measured in random-field-based lead-based relaxors, which exhibit a frequency scale of order of $\sim$GHz and are comparatively better correlated spatially. Our results support the view that random fields give rise to the relaxor phenomena, and that the glass-like dynamics observed here characterize a nascent response.

cond-mat.mtrl-sci↗

arXiv2015

Separation of magnetic and superconducting behaviour in YBCO6.33 (Tc=8.4 K)

Neutron scattering from high-quality YBa2Cu3O6.33 (YBCO6.33) single crystals with a Tc of 8.4 K shows no evidence of a coexistence of superconductivity with long-range antiferromagnetic order at this very low, near-critical doping of p~0.055. However, we find short-range three dimensional spin correlations that develop at temperatures much higher than Tc. Their intensity increases smoothly on cooling and shows no anomaly that might signify a Neel transition. The system remains subcritical with spins correlated over only one and a half unit cells normal to the planes. At low energies the short-range spin response is static on the microvolt scale. The excitations out of this ground state give rise to an overdamped spectrum with a relaxation rate of 3 meV. The transition to the superconducting state below Tc has no effect on the spin correlations. The elastic interplanar spin response extends over a length that grows weakly but fails to diverge as doping is moved towards the superconducting critical point. Any antiferromagnetic critical point likely lies outside the superconducting dome. The observations suggest that conversion from Neel long-range order to a spin glass texture is a prerequisite to formation of paired superconducting charges. We show that while pc =0.052 is a critical doping for superconducting pairing, it is not for spin order.

cond-mat.supr-con↗

arXiv2015

Spin waves and revised crystal structure of honeycomb iridate Na2IrO3

We report inelastic neutron scattering measurements on Na2IrO3, a candidate for the Kitaev spin model on the honeycomb lattice. We observe spin-wave excitations below 5 meV with a dispersion that can be accounted for by including substantial further-neighbor exchanges that stabilize zig-zag magnetic order. The onset of long-range magnetic order below 15.3 K is confirmed via the observation of oscillations in zero-field muon-spin rotation experiments. Combining single-crystal diffraction and density functional calculations we propose a revised crystal structure model with significant departures from the ideal 90 deg Ir-O-Ir bonds required for dominant Kitaev exchange.

cond-mat.str-el↗

arXiv2014

Magnetism of the Fe$^{2+}$ and Ce$^{3+}$ sublattices in Ce$_{2}$O$_{2}$FeSe$_{2}$: a combined neutron powder diffraction, inelastic neutron scattering and density functional study

The discovery of superconductivity in the 122 iron selenide materials above 30 K necessitates an understanding of the underlying magnetic interactions. We present a combined experimental and theoretical investigation of magnetic and semiconducting Ce$_{2}$O$_{2}$FeSe$_{2}$ composed of chains of edge-linked iron selenide tetrahedra. The combined neutron diffraction and inelastic scattering study and density functional calculations confirm the ferromagnetic nature of nearest-neighbour Fe -- Se -- Fe interactions in the ZrCuSiAs-related iron oxyselenide Ce$_{2}$O$_{2}$FeSe$_{2}$. Inelastic measurements provide an estimate of the strength of nearest-neighbor Fe -- Fe and Fe -- Ce interactions. These are consistent with density functional theory calculations, which reveal that correlations in the Fe--Se sheets of Ce$_{2}$O$_{2}$FeSe$_{2}$ are weak. The Fe on-site repulsion $U_{Fe}$ is comparable to that reported for oxyarsenides and K$_{1-x}$Fe$_{2-y}$Se$_{2}$, which are parents to iron-based superconductors.

cond-mat.str-el↗

arXiv2014

Neutron inelastic scattering measurements of low energy phonons in the multiferroic BiFeO3

We present neutron inelastic scattering measurements of the low-energy phonons in single crystal BiFeO3. The dispersions of the three acoustic phonon modes (LA along [100], TA1 along [010] and TA2 along [110]) and two low energy optic phonon modes (LO and TO1) have been mapped out between 300 K and 700 K. Elastic constants are extracted from the phonon measurements. The energy linewidths of both TA phonons at the zone boundary clearly broaden when the system is warmed toward the magnetic ordering temperature TN = 640 K. This suggests that the magnetic and low-energy lattice dynamics in this multiferroic material are coupled.

cond-mat.mtrl-sci↗

arXiv2014

Neutron Scattering Evidence for a Periodically-Modulated Superconducting Phase in the Underdoped Cuprate La$_{1.905}$Ba$_{0.095}$CuO$_4$

The role of antiferromagnetic spin correlations in high-temperature superconductors remains a matter of debate. We present inelastic neutron scattering evidence that gapless spin fluctuations coexist with superconductivity in La$_{1.905}$Ba$_{0.095}$CuO$_4$. Furthermore, we observe that both the low-energy magnetic spectral weight and the spin incommensurability are enhanced by the onset of superconducting correlations. We propose that the coexistence occurs through intertwining of spatial modulations of the pair wave function and the antiferromagnetic correlations. This proposal is also directly relevant to sufficiently underdoped La$_{2-x}$Sr$_x$CuO$_4$ and YBa$_2$Cu$_3$O$_{6+x}$.

cond-mat.supr-con↗

arXiv2014

Soft striped magnetic fluctuations competing with superconductivity in Fe_{1+x}Te

Neutron spectroscopy is used to investigate the magnetic fluctuations in Fe_{1+x}Te - a parent compound of chalcogenide superconductors. Incommensurate "stripe-like" excitations soften with increased interstitial iron concentration. The energy crossover from incommensurate to stripy fluctuations defines an apparent hour-glass dispersion. Application of sum rules of neutron scattering find that the integrated intensity is inconsistent with an S=1 Fe^{2+} ground state and significantly less than S=2 predicted from weak crystal field arguments pointing towards the Fe^{2+} being in a superposition of orbital states. The results suggest that a highly anisotropic order competes with superconductivity in chalcogenide systems.

cond-mat.str-el↗

arXiv2014

Excitations in the quantum paramagnetic phase of the quasi-one-dimensional Ising magnet CoNb$_2$O$_6$ in a transverse field: Geometric frustration and quantum renormalization effects

The quasi-one-dimensional (1D) Ising ferromagnet CoNb$_2$O$_6$ has recently been driven via applied transverse magnetic fields through a continuous quantum phase transition from spontaneous magnetic order to a quantum paramagnet, and dramatic changes were observed in the spin dynamics, characteristic of weakly perturbed 1D Ising quantum criticality. We report here extensive single-crystal inelastic neutron scattering measurements of the magnetic excitations throughout the three-dimensional (3D) Brillouin zone in the quantum paramagnetic phase just above the critical field to characterize the effects of the finite interchain couplings. In this phase, we observe that excitations have a sharp, resolution-limited line shape at low energies and over most of the dispersion bandwidth, as expected for spin-flip quasiparticles. We map the full bandwidth along the strongly dispersive chain direction and resolve clear modulations of the dispersions in the plane normal to the chains, characteristic of frustrated interchain couplings in an antiferromagnetic isosceles triangular lattice. The dispersions can be well parametrized using a linear spin-wave model that includes interchain couplings and further neighbor exchanges. The observed dispersion bandwidth along the chain direction is smaller than that predicted by a linear spin-wave model using exchange values determined at zero field, and this effect is attributed to quantum renormalization of the dispersion beyond the spin-wave approximation in fields slightly above the critical field, where quantum fluctuations are still significant.

cond-mat.str-el↗

arXiv2014

The role of random electric fields in relaxors

PbZr_{1-x}Ti_xO_3 (PZT) and Pb(Mg_{1/3}Nb_{2/3})_{1-x}Ti_xO_3 (PMN-$x$PT) are complex lead-oxide perovskites that display exceptional piezoelectric properties for pseudorhombohedral compositions near a tetragonal phase boundary. In PZT these compositions are ferroelectrics, but in PMN-xPT they are relaxors because the dielectric permittivity is frequency dependent and exhibits non-Arrhenius behavior. We show that the nanoscale structure unique to PMN-xPT and other lead-oxide perovskite relaxors is absent in PZT and correlates with a greater than 100% enhancement of the longitudinal piezoelectric coefficient in PMN-xPT relative to that in PZT. By comparing dielectric, structural, lattice dynamical, and piezoelectric measurements on PZT and PMN-xPT, two nearly identical compounds that represent weak and strong random electric field limits, we show that quenched (static) random fields establish the relaxor phase and identify the order parameter.

cond-mat.mtrl-sci↗

arXiv2014

Weak spin interactions in Mott insulating La2O2Fe2OSe2

Identifying and characterizing the parent phases of iron-based superconductors is an important step towards understanding the mechanism for their high temperature superconductivity. We present an investigation into the magnetic interactions in the Mott insulator La2O2Fe2OSe2. This iron oxyselenide adopts a 2-k magnetic structure with low levels of magnetic frustration. This magnetic ground state is found to be dominated by next-nearest neighbor interactions J2 and J2' and the magnetocrystalline anisotropy of the Fe2+ site, leading to 2D-Ising-like spin S=2 fluctuations. In contrast to calculations, the values are small and confine the spin excitations below ~ 25 meV. This is further corroborated by sum rules of neutron scattering. This indicates that superconductivity in related materials may derive from a weakly coupled and unfrustrated magnetic structure.

cond-mat.str-el↗

arXiv2013

Neutron scattering measurements of $dd$ and spin-orbit excitations below the Mott-Hubbard gap in CoO

Neutron scattering is used to investigate the single-ion spin and orbital excitations below the Mott-Hubbard gap in CoO. Three excitations are reported at 0.870 $\pm$ 0.009 eV, 1.84 $\pm$ 0.03, and 2.30 $\pm$ 0.15 eV. These were parameterized within a weak crystal field scheme with an intra-orbital exchange of $J(dd)$=1.3 $\pm$ 0.2 eV and a crystal field splitting 10Dq=0.94 $\pm$ 0.10 eV. A reduced spin-orbit coupling of λ=-0.016 $\pm$ 0.003 eV is derived from dilute samples of Mg$_{0.97}$Co$_{0.03}$O, measured to remove complications due to spin exchange and structural distortion parameters which split the cubic phase degeneracy of the orbital excitations complicating the inelastic spectrum. The 1.84 eV, while reported using resonant x-ray and optical techniques, was absent or weak for non resonant x-ray experiments and overlaps with the expected position of a $^{4}A_{2}$ level. This transition is absent in the dipolar approximation but expected to have a finite quadrupolar matrix element that can be observed with neutron scattering techniques at larger momentum transfers. Our results agree with a crystal field analysis (in terms of Racah parameters and Tanabe-Sugano diagrams) and with previous calculations performed using local-density band theory for Mott insulating transition metal oxides. The results also demonstrate the use of neutron scattering for measuring dipole forbidden transitions in transition metal oxide systems.

cond-mat.str-el↗

arXiv2013

Coupled magnetic and ferroelectric excitations in PbFe_{1/2}Nb_{1/2}O_{3}

A neutron scattering investigation of the magnetoelectric coupling in PbFe_{1/2}Nb_{1/2}O_{3} (PFN) has been undertaken. Ferroelectric order occurs below 400 K, as evidenced by the softening with temperature and subsequent recovery of the zone center transverse optic phonon mode energy (\hbar Ω_{0}). Over the same temperature range, magnetic correlations become resolution limited on a terahertz energy scale. In contrast to the behavior of nonmagnetic disordered ferroelectrics (namely Pb(Mg,Zn)_{1/3}Nb_{2/3}O_{3}), we report the observation of a strong deviation from linearity in the temperature dependence of (\hbar Ω_{0})^{2}. This deviation is compensated by a corresponding change in the energy scale of the magnetic excitations, as probed through the first moment of the inelastic response. The coupling between the short-range ferroelectric and antiferromagnetic correlations is consistent with calculations showing that the ferroelectricity is driven by the displacement of the body centered iron site, illustrating the multiferroic nature of magnetic lead based relaxors in the dynamical regime.

cond-mat.mtrl-sci↗

arXiv2013

The magnetic and structural properties near the Lifshitz point in Fe1+xTe

We construct a phase diagram of the parent compound Fe1+xTe as a function of interstitial iron x in terms of the electronic, structural, and magnetic properties. For a concentration of x < 10%, Fe1+xTe undergoes a "semimetal" to metal transition at approximately 70 K that is also first-order and coincident with a structural transition from a tetragonal to a monoclinic unit cell. For x ~ 14%, Fe1+xTe undergoes a second-order phase transition at approximately 58 K corresponding to a "semimetal" to "semimetal" transition along with a structural orthorhombic distortion. At a critical concentration of x ~ 11%, Fe1+xTe undergoes two transitions: the higher temperature one is a second-order transition to an orthorhombic phase with incommensurate magnetic ordering and temperature-dependent propagation vector, while the lower temperature one corresponds to nucleation of a monoclinic phase with a nearly commensurate magnetic wavevector. While both structural and magnetic transitions display similar critical behavior for x < 10% and near the critical concentration of x ~ 11%, samples with large interstitial iron concentrations show a marked deviation between the critical response indicating a decoupling of the order parameters. Analysis of temperature dependent inelastic neutron data reveals incommensurate magnetic fluctuations throughout the Fe1+xTe phase diagram are directly connected to the "semiconductor"-like resistivity above T_N and implicates scattering from spin fluctuations as the primary reason for the semiconducting or poor metallic properties. The results suggest that doping driven Fermi surface nesting maybe the origin of the gapless and incommensurate spin response at large interstitial concentrations.

cond-mat.str-el↗

arXiv2012

Evidence for anisotropic polar nanoregions in relaxor PMN: A neutron study of the elastic constants and anomalous TA phonon damping

We use neutron scattering to characterize the acoustic phonons in the relaxor PMN and demonstrate the presence of an anisotropic damping mechanism directly related to short-range, polar correlations. For a large range of temperatures above Tc ~ 210, K, where dynamic polar correlations exist, acoustic phonons propagating along [1\bar{1}0] and polarized along [110] (TA2 phonons) are overdamped and softened across most of the Brillouin zone. By contrast, acoustic phonons propagating along [100] and polarized along [001] (TA1 phonons) are overdamped and softened for only a limited range of wavevectors. The anisotropy and temperature dependence of the acoustic phonon energy linewidth are directly correlated with the elastic diffuse scattering, 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, 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 and to values reported for pure PT. We show that while the values of C44 are quite similar, those for C11 and C12 are significantly less in PMN and result in a softening of (C11-C12) over PT. There is also an increased elastic anisotropy (2C44/(C11-C12)) versus that in PT. These results suggest an instability to TA2 acoustic fluctuations in relaxors. We discuss our results in the context of the debate over the "waterfall" effect and show that they are inconsistent with TA-TO phonon coupling or other models that invoke the presence of a second optic mode.

cond-mat.mtrl-sci↗