Karol Marty

Giant anharmonic phonon scattering in PbTe

Understanding the microscopic processes affecting the bulk thermal conductivity is crucial to develop more efficient thermoelectric materials. PbTe is currently one of the leading thermoelectric materials, largely thanks to its low thermal conductivity. However, the origin of this low thermal conductivity in a simple rocksalt structure has so far been elusive. Using a combination of inelastic neutron scattering measurements and first-principles computations of the phonons, we identify a strong anharmonic coupling between the ferroelectric transverse optic mode and the longitudinal acoustic modes in PbTe. This interaction extends over a large portion of reciprocal space, and directly affects the heat-carrying longitudinal acoustic phonons. The longitudinal acoustic-transverse optic anharmonic coupling is likely to play a central role in explaining the low thermal conductivity of PbTe. The present results provide a microscopic picture of why many good thermoelectric materials are found near a lattice instability of the ferroelectric type.

Phonon softening and metallization of a narrow-gap semiconductor by thermal disorder

The vibrations of ions in solids at finite temperature depend on interatomic force–constants that result from electrostatic interactions between ions, and the response of the electron density to atomic displacements. At high temperatures, vibration amplitudes are substantial, and electronic states are affected, thus modifying the screening properties of the electron density. By combining inelastic neutron scattering measurements of Fe1-xCoxSi as a function of temperature, and finite-temperature first-principles calculations including thermal disorder effects, we show that the coupling between phonons and electronic structure results in an anomalous temperature dependence of phonons. The strong concomitant renormalization of the electronic structure induces the semiconductor-to-metal transition that occurs with increasing temperature in FeSi. Our results show that for systems with rapidly changing electronic densities of states at the Fermi level, there are likely to be significant phonon–electron interactions, resulting in anomalous temperature-dependent properties.

Single domain magnetic helicity and triangular chirality in structurally enantiopure Ba3NbFe3Si2O14.

A novel doubly chiral magnetic order is found in the structurally chiral langasite compound Ba3NbFe3Si2O14. The magnetic moments are distributed over planar frustrated triangular lattices of triangle units. On each of these they form the same triangular configuration. This ferrochiral arrangement is helically modulated from plane to plane. Unpolarized neutron scattering on a single crystal associated with spherical neutron polarimetry proved that a single triangular chirality together with a single helicity is stabilized in an enantiopure crystal. A mean-field analysis allows us to discern the relevance on this selection of a twist in the plane to plane super-superexchange paths.

Competing ferri- and antiferromagnetic phases in geometrically frustrated LuFe2O4.

We present a detailed study of magnetism in LuFe(2)O(4), combining magnetization measurements with neutron and soft x-ray diffraction. The magnetic phase diagram in the vicinity of T(N) involves a metamagnetic transition separating an antiferro- and a ferrimagnetic phase. For both phases the spin structure is refined by neutron diffraction. Observed diffuse magnetic scattering far above T(N) is explained in terms of near degeneracy of the magnetic phases.

Electron-doping evolution of the low-energy spin excitations in the iron arsenide superconductor BaFe2-xNixAs2

BaFe1.9Ni0.1As2 Tc =2 0 K and overdoped BaFe1.85Ni0.15As2 Tc =1 4 K superconductors, the static AF longrange order is completely suppressed and the spin excitation spectra are dominated by a resonance and spin gap at lower energies. We determine the electron-doping dependence of the neutron spin resonance and spin gap energies and demonstrate that the three-dimensional nature of the resonance survives into the overdoped regime. If spin excitations are important for superconductivity, these results would suggest that the threedimensional characters of the electronic superconducting gaps are prevalent throughout the phase diagram and may be critical for superconductivity in these materials.

Neutron Scattering Studies of spin excitations in hole-doped Ba0.67K0.33Fe2As2 superconductor

We report inelastic neutron scattering experiments on single crystals of superconducting Ba0.67K0.33Fe2As2 (Tc = 38 K). In addition to confirming the resonance previously found in powder samples, we find that spin excitations in the normal state form longitudinally elongated ellipses along the QAFM direction in momentum space, consistent with density functional theory predictions. On cooling below Tc, while the resonance preserves its momentum anisotropy as expected, spin excitations at energies below the resonance become essentially isotropic in the in-plane momentum space and dramatically increase their correlation length. These results suggest that the superconducting gap structures in Ba0.67Ka0.33Fe2As2 are more complicated than those suggested from angle resolved photoemission experiments.

Competing magnetic ground states in nonsuperconducting Ba(Fe1-xCrx)2As2 as seen via neutron diffraction

We present neutron diffraction measurements on single-crystal samples of nonsuperconducting Ba(Fe{sub 1-x}Cr{sub x}){sub 2}As{sub 2} as a function of Cr doping for 0 x 0.47. The average spin-density-wave moment is independent of concentration for x 0.2 and decreases rapidly for x 0.3. For concentrations in excess of 30% chromium, we find a new competing magnetic phase consistent with G-type antiferromagnetism which rapidly becomes the dominant magnetic ground state. Strong magnetism is observed for all concentrations measured, naturally explaining the absence of superconductivity in the Cr-doped materials.

Direct observation of dynamic charge stripes in La2–xSrxNiO4

The insulator-to-metal transition continues to be a challenging subject, especially when electronic correlations are strong. In layered compounds, such as La2-xSrxNiO4 and La2-xBaxCuO4, the doped charge carriers can segregate into periodically spaced charge stripes separating narrow domains of antiferromagnetic order. Although there have been theoretical proposals of dynamically fluctuating stripes, direct spectroscopic evidence of charge-stripe fluctuations has been lacking. Here we report the detection of critical lattice fluctuations, driven by charge-stripe correlations, in La2-xSrxNiO4 using inelastic neutron scattering. This scattering is detected at large momentum transfers where the magnetic form factor suppresses the spin fluctuation signal. The lattice fluctuations associated with the dynamic charge stripes are narrow in q and broad in energy. They are strongest near the charge-stripe melting temperature. Our results open the way towards the quantitative theory of dynamic stripes and for directly detecting dynamical charge stripes in other strongly correlated systems, including high-temperature superconductors such as La2-xSrxCuO4.

Effects of Transition Metal Substitutions on the Incommensurability and Spin Fluctuations in BaFe2As2 by Elastic and Inelastic Neutron Scattering

The spin fluctuation spectra from nonsuperconducting Cu-substituted, and superconducting Co-substituted, BaFe(2)As(2) are compared quantitatively by inelastic neutron scattering measurements and are found to be indistinguishable. Whereas diffraction studies show the appearance of incommensurate spin-density wave order in Co and Ni substituted samples, the magnetic phase diagram for Cu substitution does not display incommensurate order, demonstrating that simple electron counting based on rigid-band concepts is invalid. These results, supported by theoretical calculations, suggest that substitutional impurity effects in the Fe plane play a significant role in controlling magnetism and the appearance of superconductivity, with Cu distinguished by enhanced impurity scattering and split-band behavior.

Effect of molybdenum 4d hole substitution in BaFe2As2

We investigate the thermodynamic and transport properties of molybdenum-doped BaFe2As2 (122) crystals, the first report of hole doping using a 4d element. The chemical substitution of Mo in place of Fe is possible up to {approx} 7%. For Ba(Fe1-xMox)2As2, the suppression rate of the magnetic transition temperature with x is the same as in 3d Cr-doped 122 and is independent of the unit cell changes. This illustrates that the temperature-composition phase diagram for hole-doped 122 can be simply parameterized by x, similar to the electron-doped 122 systems found in the literature. Compared to 122 with a coupled antiferromagnetic order (TN) and orthorhombic structural transition (T0) at {approx}132 K, 1.3% Mo-doped 122 (x=0.013) gives TN=T0=125(1) K according to neutron diffraction results and features in specific heat, magnetic susceptibility, and electrical resistivity. The cell volume expands by {approx}1% with maximum Mo doping and TN is reduced to {approx}90 K. There is a T* feature that is identified for lightly Cr- or Mo-doped 122 crystals, which is x dependent. This low-temperature transition may be a trace of superconductivity.