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J. W. Lynn

Publications and source records attributed to J. W. Lynn.

At least 55 records · Page 3Linked to original sources

Magnetic neutron diffraction study of Ba(Fe1-xCox)2As2 critical exponents through the tricritical doping

We present temperature dependent magnetic neutron diffraction measurements on Ba(Fe$_{1-x}$Co$_{x}$)$_{2}$As$_{2}$ for $x$ = 0.039, 0.022, and 0.021 as-grown single crystals. Our investigations probe the behavior near the magnetic tricritical point in the ($x$,$T$) plane, $x_{tr} \approx $0.022, as well as systematically exploring the character of the magnetic phase transition across a range of doping values. All samples show long range antiferromagnetic order that may be described near the transition by simple power laws, with $β$ =~0.306$\pm$0.060 for $x$ =~0.039, $β$ =~0.208$\pm$0.005 for $x$ =~0.022, and $β$ =~0.198$\pm$0.009 for $x$ =~0.021. For the $x$ =~0.039 sample, the data are reasonably well described by the order parameter exponent $β$ =~0.326 expected for a 3D Ising model while the $x$ =~0.022 and $x$ =~0.021 samples are near the $β$ =~0.25 value for a tricritical system in the mean-field approximation. These results are discussed in the context of existing experimental work and theoretical predictions.

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Two-Dimensional Magnetic Correlations and Partial Long-Range Order in Geometrically Frustrated Sr2YRuO6

Neutron diffraction on the double perovskite Sr2YRuO6 with a quasi-face-centered cubic (FCC) lattice of Ru moments reveals planar magnetic correlations that condense into a partial long-range ordered state with coupled alternate antiferromagnetic (AFM) YRuO4 square layers coexisting with short-range correlations below T{N1}=32 K. A second transition to a fully ordered AFM state below T{N2}=24 K is observed. These observations are ascribed to the cancellation of the magnetic coupling between consecutive AFM square layers in FCC antiferromagnets, notably the simplest three-dimensional frustrated magnet model system. Inhomogeneous superconductivity in Sr2YRu_{1-x}Cu_{x}O6, reported in earlier works, may be nucleated in magnetically disordered YRu_{1-x}Cu_{x}O4 layers with strong spin fluctuations.

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Tuning magnetism in FeAs-based materials via tetrahedral structure

Resistivity, magnetic susceptibility, neutron scattering and x-ray crystallography measurements were used to study the evolution of magnetic order and crystallographic structure in single-crystal samples of the Ba1-xSrxFe2As2 and Sr1-yCayFe2As2 series. A non-monotonic dependence of the magnetic ordering temperature T0 on chemical pressure is compared to the progression of the antiferromagnetic staggered moment, characteristics of the ordering transition and structural parameters to reveal a distinct relationship between the magnetic energy scale and the tetrahedral bond angle, even far above T0. In Sr1-yCayFe2As2, an abrupt drop in T0 precisely at the Ca concentration where the tetrahedral structure approaches the ideal geometry indicates a strong coupling between the orbital bonding structure and the stabilization of magnetic order, providing strong constraints on the nature of magnetism in the iron-arsenide superconducting parent compounds.

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Field-induced quantum fluctuations in the heavy fermion superconductor CeCu2Ge2

Quantum-mechanical fluctuations in strongly correlated electron systems cause unconventional phenomena such as non-Fermi liquid behavior, and arguably high temperature superconductivity. Here we report the discovery of a field-tuned quantum critical phenomenon in stoichiometric CeCu2Ge2, a spin density wave ordered heavy fermion metal that exhibits unconventional superconductivity under ~ 10 GPa of applied pressure. Our finding of the associated quantum critical spin fluctuations of the antiferromagnetic spin density wave order, dominating the local fluctuations due to single-site Kondo effect, provide new information about the underlying mechanism that can be important in understanding superconductivity in this novel compound.

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Multiple Magnetic Structures of Correlated Ce-ions in Intermetallic CeAu2Ge2

Neutron diffraction measurements on a high quality single crystal of CeAu2Ge2 reveal two new magnetic structures that coexist with commensurate long range antiferromagnetic order below the Neel temperature T_N ~ 14 K. The new magnetic structures, which exhibit distinct temperature and field dependencies, are described by both commensurate and incommensurate magnetic structures and introduces new region in the H-T phase diagram. These new experimental observations provide essential information for developing a universal understanding of the magnetic properties of this class of Ce-based CeX2M2 (X = Cu, Ag, Au; M = Ge, Si) compounds, which are prototypes for exploring quantum phase transitions and their interplay with unconventional superconductivity.

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Structural collapse and superconductivity in rare earth-doped CaFe2As2

Aliovalent rare earth substitution into the alkaline earth site of CaFe2As2 single-crystals is used to fine-tune structural, magnetic and electronic properties of this iron-based superconducting system. Neutron and single crystal x-ray scattering experiments indicate that an isostructural collapse of the tetragonal unit cell can be controllably induced at ambient pressures by choice of substituent ion size. This instability is driven by the interlayer As-As anion separation, resulting in an unprecedented thermal expansion coefficient of $180\times 10^{-6}$ K$^{-1}$. Electrical transport and magnetic susceptibility measurements reveal abrupt changes in the physical properties through the collapse as a function of temperature, including a reconstruction of the electronic structure. Superconductivity with onset transition temperatures as high as 47 K is stabilized by the suppression of antiferromagnetic order via chemical pressure, electron doping or a combination of both. Extensive investigations are performed to understand the observations of partial volume-fraction diamagnetic screening, ruling out extrinsic sources such as strain mechanisms, surface states or foreign phases as the cause of this superconducting phase that appears to be stable in both collapsed and uncollapsed structures.

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Response of acoustic phonons to charge and orbital order in the 50\% doped bilayer manganite LaSr$_2$Mn$_2$O$_7$

We report an inelastic neutron scattering study of acoustic phonons in the charge and orbitally ordered bilayer manganite LaSr$_2$Mn$_2$O$_7$. For excitation energies less than $15\,\rm{meV}$, we observe an abrupt increase (decrease) of the phonon energies (linewidths) of a transverse acoustic phonon branch at $\mathbf{q} = (h, h, 0)$, $h\le0.3$, upon entering the low temperature charge and orbital ordered state ($T_{COO} = 225\,\rm{K}$). This indicates a reduced electron-phonon coupling due to a decrease of electronic states at the Fermi level leading to a partial removal of the Fermi surface below $T_{COO}$ and provides direct experimental evidence for a link between electron-phonon coupling and charge order in manganites.

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From antiferromagnetic insulator to correlated metal in pressurized and doped LaMnPO

Widespread adoption of superconducting technologies requires the discovery of new materials with enhanced properties, especially higher superconducting transition temperatures T$_{c}$. The unexpected discovery of high T$_{c}$ superconductivity in cuprates and in materials as diverse as heavy fermions, organic conductors, and endohedrally-doped fullerenes suggests that the highest T$_{c}$s occur when pressure or doping transform the localized and moment-bearing electrons in antiferromagnetic insulators into itinerant and weakly magnetic metals. The absence of this delocalization transition in Fe-based superconductors may limit their T$_{c}$s, but even larger T$_{c}$s may be possible in their isostructural Mn analogs, which are antiferromagnetic insulators like the cuprates. It is generally believed that prohibitively large pressures would be required to suppress the strong Hund's rule coupling in these Mn-based compounds, collapsing the insulating gap and enabling superconductivity. Indeed, no Mn-based compounds are known to be superconductors. The electronic structure calculations and x-ray diffraction measurements presented here challenge these long held beliefs, finding that only modest pressures are required to transform LaMnPO, isostructural to superconducting host LaFeAsO, from an insulating tetragonal structure with a large Mn moment to a gapless orthorhombic structure with a small Mn moment. Proximity to this electronic delocalization transition in LaMnPO results in a highly interacting metallic state, the familiar breeding ground of superconductivity.

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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.

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Common origin of the two types of magnetic fluctuations in iron chalcogenides

We use inelastic neutron scattering to study the low energy spin excitations in moderately doped non-superconducting Fe$_{1.01}$Te$_{0.72}$Se$_{0.28}$. The spin excitations in this system contain components near (0.5,0,0) and (0.5,0.5,0) in a-b plane reciprocal lattice units using tetragonal unit cell notation (a=b=3.772 Åand c=6.061 Å). At low energies the scattering is centered around (0.5,0,0). With increasing energy, the spectral weight of low energy spin excitations centered around (0.5,0,0) abruptly shifts around 3 meV to the incommensurate spin excitations centered around (0.5,0.5,0). However both types of spin fluctuations exhibit the identical temperature dependence. These results indicate that the (0.5,0,0) type spin excitations and the incommensurate excitations around the (0.5,0.5,0) position have a common origin and both must be taken into account to understand the nature of magnetism and superconducting pairing in the iron chalcogenides.

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Antiferromagnetic order and superlattice structure in nonsuperconducting and superconducting RbyFe(1.6+x)Se2

Neutron diffraction has been used to study the lattice and magnetic structures of the insulating and superconducting Rb$_y$Fe$_{1.6+x}$Se$_2$. For the insulating Rb$_{y}$Fe$_{1.6+x}$Se$_2$, neutron polarization analysis and single crystal neutron diffraction unambiguously confirm the earlier proposed $\sqrt{5}\times\sqrt{5}$ block antiferromagnetic structure. For superconducting samples ($T_c=30$ K), we find that in addition to the tetragonal $\sqrt{5}\times\sqrt{5}$ superlattice structure transition at 513 K, the material develops a separate $\sqrt{2}\times \sqrt{2}$ superlattice structure at a lower temperature of 480 K. These results suggest that superconducting Rb$_{y}$Fe$_{1.6+x}$Se$_2$ is phase separated with coexisting $\sqrt{2}\times \sqrt{2}$ and $\sqrt{5}\times\sqrt{5}$ superlattice structures.

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Magnetic field tuning of antiferromagnetic Yb$_{3}$Pt$_{4}$

We present measurements of the specific heat, magnetization, magnetocaloric effect and magnetic neutron diffraction carried out on single crystals of antiferromagnetic Yb$_{3}$Pt$_{4}$, where highly localized Yb moments order at $T_{\rm N}=2.4$ K in zero field. The antiferromagnetic order was suppressed to $T_{\rm N}\rightarrow 0$ by applying a field of 1.85 T in the $ab$ plane. Magnetocaloric effect measurements show that the antiferromagnetic phase transition is always continuous for $T_{\rm N}>0$, although a pronounced step in the magnetization is observed at the critical field in both neutron diffraction and magnetization measurements. These steps sharpen with decreasing temperature, but the related divergences in the magnetic susceptibility are cut off at the lowest temperatures, where the phase line itself becomes vertical in the field-temperature plane. As $T_{\rm N}\rightarrow0$, the antiferromagnetic transition is increasingly influenced by a quantum critical endpoint, where $T_{\rm N}$ ultimately vanishes in a first order phase transition.

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Antiferromagnetic spin excitations in single crystals of nonsuperconducting Li1-xFeAs

We use neutron scattering to determine spin excitations in single crystals of nonsuperconducting Li1-xFeAs throughout the Brillouin zone. Although angle resolved photoemission experiments and local density approximation calculations suggest poor Fermi surface nesting conditions for antiferromagnetic(AF) order, spin excitations in Li1-xFeAs occur at the AF wave vectors Q = (1, 0) at low energies, but move to wave vectors Q = (\pm 0.5, \pm0.5) near the zone boundary with a total magnetic bandwidth comparable to that of BaFe2As2. These results reveal that AF spin excitations still dominate the low-energy physics of these materials and suggest both itinerancy and strong electron-electron correlations are essential to understand the measured magnetic excitations.

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Quantum critical behavior in the heavy Fermion single crystal Ce(Ni$_{0.935}$Pd$_{0.065}$)$_2$Ge$_2$

We have performed magnetic susceptibility, specific heat, resistivity, and inelastic neutron scattering measurements on a single crystal of the heavy Fermion compound Ce(Ni$_{0.935}$Pd$_{0.065}$)$_2$Ge$_2$, which is believed to be close to a quantum critical point (QCP) at T = 0. At lowest temperature(1.8-3.5 K), the magnetic susceptibility behaves as $χ(T)-χ(0)$ $\propto$ $T^{-1/6}$ with $χ(0) = 0.032 \times 10^{-6}$ m$^3$/mole (0.0025 emu/mole). For $T<$ 1 K, the specific heat can be fit to the formula $ΔC/T = γ_0 - T^{1/2}$ with $γ_0$ of order 700 mJ/mole-K$^2$. The resistivity behaves as $ρ= ρ_0 + AT^{3/2}$ for temperatures below 2 K. This low temperature behavior for $γ(T)$ and $ρ(T)$ is in accord with the SCR theory of Moriya and Takimoto\cite{Moriya}. The inelastic neutron scattering spectra show a broad peak near 1.5 meV that appears to be independent of $Q$; we interpret this as Kondo scattering with $T_K =$ 17 K. In addition, the scattering is enhanced near $Q$=(1/2, 1/2, 0) with maximum scattering at $ΔE$ = 0.45 meV; we interpret this as scattering from antiferromagnetic fluctuations near the antiferromagnetic QCP.

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Molecular spin-orbit excitations in the J_eff = 1/2 frustrated spinel GeCo$_2$O$_4$

We describe powder and single-crystal inelastic neutron scattering experiments on a spinel-type antiferromagnet GeCo$_2$O$_4$, represented by an effective total angular momentum J_eff = 1/2. Several types of non-dispersive short-range magnetic excitations were discovered. The scattering intensity maps in $\vec{Q}$ space are well reproduced by dynamical structure factor analyses using molecular model Hamiltonians. The results of analyses strongly suggest that the molecular excitations below T_N arise from a hidden molecular-singlet ground state, in which ferromagnetic subunits are antiferromagnetically coupled. The quasielastic excitations above T_N are interpreted as its precursor. A combination of frustration and J_eff = 1/2 might induce these quantum phenomena.

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Dzyaloshinskii-Moriya interaction and spin re-orientation transition in the frustrated kagome lattice antiferromagnet

Magnetization, specific heat, and neutron scattering measurements were performed to study a magnetic transition in jarosite, a spin-5/2 kagome lattice antiferromagnet. When a magnetic field is applied perpendicular to the kagome plane, magnetizations in the ordered state show a sudden increase at a critical field H_c, indicative of the transition from antiferromagnetic to ferromagnetic states. This sudden increase arises as the spins on alternate kagome planes rotate 180 degrees to ferromagnetically align the canted moments along the field direction. The canted moment on a single kagome plane is a result of the Dzyaloshinskii-Moriya interaction. For H < H_c, the weak ferromagnetic interlayer coupling forces the spins to align in such an arrangement that the canted components on any two adjacent layers are equal and opposite, yielding a zero net magnetic moment. For H > H_c, the Zeeman energy overcomes the interlayer coupling causing the spins on the alternate layers to rotate, aligning the canted moments along the field direction. Neutron scattering measurements provide the first direct evidence of this 180-degree spin rotation at the transition.

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Antiferromagnetic Critical Fluctuations in BaFe$_2$As$_2$

Magnetic correlations near the magneto-structural phase transition in the bilayer iron pnictide parent compound, BaFe$_2$As$_2$, are measured. In close proximity to the antiferromagnetic phase transition in BaFe$_2$As$_2$, a crossover to three dimensional critical behavior is anticipated and has been preliminarily observed. Here we report complementary measurements of two-dimensional magnetic fluctuations over a broad temperature range about T$_N$. The potential role of two-dimensional critical fluctuations in the magnetic phase behavior of BaFe$_2$As$_2$ and their evolution near the anticipated crossover to three dimensional critical behavior and long-range order are discussed.

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Doping Dependence of Spin Dynamics in Electron-Doped Ba(Fe1-xCox)2As2

The spin dynamics in single crystal, electron-doped Ba(Fe1-xCox)2As2 has been investigated by inelastic neutron scattering over the full range from undoped to the overdoped regime. We observe damped magnetic fluctuations in the normal state of the optimally doped compound (x=0.06) that share a remarkable similarity with those in the paramagnetic state of the parent compound (x=0). In the overdoped superconducting compound (x=0.14), magnetic excitations show a gap-like behavior, possibly related to a topological change in the hole Fermi surface (Lifshitz transition), while the imaginary part of the spin susceptibility prominently resembles that of the overdoped cuprates. For the heavily overdoped, non-superconducting compound (x=0.24) the magnetic scattering disappears, which could be attributed to the absence of a hole Fermi-surface pocket observed by photoemission.

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