arXiv subjects

M. D. Lumsden

Publications and source records attributed to M. D. Lumsden.

At least 37 records · Page 2Linked to original sources

arXiv2016

Extended Magnetic Exchange Interactions in the High-Temperature Ferromagnet MnBi

The high-temperature ferromagnet MnBi continues to receive attention as a candidate to replace rare-earth-containing permanent magnets in applications above room temperature. This is due to a high Curie temperature, large magnetic moments, and a coercivity that increases with temperature. The synthesis of MnBi also allows for crystals that are free of interstitial Mn, enabling more direct access to the key interactions underlying the physical properties of binary Mn-based ferromagnets. In this work, we use inelastic neutron scattering to measure the spin waves of MnBi in order to characterize the magnetic exchange at low temperature. Consistent with the spin reorientation that occurs below 140 K, we do not observe a spin gap in this system above our experimental resolution. A Heisenberg model was fit to the spin wave data in order to characterize the long-range nature of the exchange. It was found that interactions up to sixth nearest neighbor are required to fully parameterize the spin waves. Surprisingly, the nearest-neighbor term is antiferromagnetic, and the realization of a ferromagnetic ground state relies on the more numerous ferromagnetic terms beyond nearest neighbor, suggesting that the ferromagnetic ground state arises as a consequence of the long-ranged interactions in the system.

cond-mat.str-el↗

arXiv2016

Comments on 'Phonon and magnetic structure in δ-plutonium from density-functional theory' by P. Söderlind et al

In their recent paper [Söderlind, P. et al., Sci. Rep. 5, 15958 (2015)], Söderlind et al. discuss two subjects from a theoretical point of view: the phonon spectra and the possible magnetic structure of δ-plutonium (Pu). Here, we comment on the second subject. Söderlind et al. compare the Pu magnetic form factor F(Q) calculated via density functional theory (DFT) with measurements of F(Q) by neutron spectroscopy [Janoschek, M. et al., Sci. Adv. 1, e1500188 (2015)]. In particular, this comparison does not consider a number of experimental facts established in the neutron spectroscopy study.

cond-mat.str-el↗

arXiv2016

Anisotropic exchange within decoupled tetrahedra in the quantum breathing pyrochlore Ba3Yb2Zn5O11

The low energy spin excitation spectrum of the breathing pyrochlore Ba3Yb2Zn5O11 has been investigated with inelastic neutron scattering. Several nearly resolution limited modes with no observable dispersion are observed at 250 mK while, at elevated temperatures, transitions between excited levels become visible. To gain deeper insight, a theoretical model of isolated Yb3+ tetrahedra parametrized by four anisotropic exchange constants is constructed. The model reproduces the inelastic neutron scattering data, specific heat, and magnetic susceptibility with high fidelity. The fitted exchange parameters reveal a Heisenberg antiferromagnet with a very large Dzyaloshinskii-Moriya interaction. Using this model, we predict the appearance of an unusual octupolar paramagnet at low temperatures and speculate on the development of inter-tetrahedron correlations.

cond-mat.str-el↗

arXiv2015

Structural and Magnetic Phase Transitions in CeCu$_{6-x}T_x$ ($T$ = Ag, Pd)

The structural and the magnetic properties of CeCu$_{6-x}$Ag$_x$ (0 $\leq$ $x$ $\leq$ 0.85) and CeCu$_{6-x}$Pd$_x$ (0 $\leq$ $x$ $\leq$ 0.4) have been studied using neutron diffraction, resonant ultrasound spectroscopy (RUS), heat capacity, x-ray diffraction measurements and first principles calculations. The structural and magnetic phase diagrams of CeCu$_{6-x}$Ag$_x$ and CeCu$_{6-x}$Pd$_x$ as a function of Ag/Pd composition are reported. The end member, CeCu$_6$, undergoes a structural phase transition from an orthorhombic ($Pnma$) to a monoclinic ($P2_1/c$) phase at 240 K. In CeCu$_{6-x}$Ag$_x$, the structural phase transition temperature (${T_{s}}$) decreases linearly with Ag concentration and extrapolates to zero at $x_{S}$ $\approx$ 0.1. The structural transition in CeCu$_{6-x}$Pd$_x$ remains unperturbed with Pd substitution within the range of our study. The lattice constant $b$ slightly decreases with Ag/Pd doping, whereas, $a$ and $c$ increase with an overall increase in the unit cell volume. Both systems, CeCu$_{6-x}$Ag$_x$ and CeCu$_{6-x}$Pd$_x$, exhibit a magnetic quantum critical point (QCP), at $x$ $\approx$ 0.2 and $x$ $\approx$ 0.05 respectively. Near the QCP, long range antiferromagnetic ordering takes place at an incommensurate wave vector ($δ_1$ 0 $δ_2$) where $δ_1 \sim 0.62$, $δ_2 \sim 0.25$, $x$ = 0.125 for CeCu$_{6-x}$Pd$_x$ and $δ_1 \sim 0.64$, $δ_2 \sim 0.3$, $x$ = 0.3 for CeCu$_{6-x}$Ag$_x$. The magnetic structure consists of an amplitude modulation of the Ce-moments which are aligned along the $c$-axis of the orthorhombic unit cell.

cond-mat.str-el↗

arXiv2015

On the Chemistry and Physical Properties of Flux and Floating Zone Grown SmB6 Single Crystals

Recent theoretical and experimental findings suggest that the long-known but not well understood low temperature resistance plateau of SmB6 may originate from protected surface states arising from a topologically non-trivial bulk band structure having strong Kondo hybridization. Yet other studies have ascribed this feature to impurity phases, sample vacancies, and surface reconstructions. Given the typical methods used to prepare SmB6 single crystals, the flux and floating zone procedures, these ascriptions should not be taken lightly. Here, we demonstrate how compositional variations and observable amounts of impurity phases in SmB6 crystals grown by floating zone and flux affect the physical properties. From neutron diffraction and X-ray computed tomography experiments, we observe that a 154Sm11B6 crystal prepared using aluminum flux contains co-crystallized, epitaxial aluminum. A large, nearly stoichiometric crystal of SmB6 was successfully grown using the float-zone technique; upon continuing the zone melting, samarium vacancies are introduced. These samarium vacancies drastically alter the resistance and plateauing magnitude of the low temperature resistance compared to stoichiometric SmB6. These results highlight that small presences of impurity phases and compositional variations must be considered when collecting and analyzing physical property data of SmB6. Finally, a more accurate samarium-154 coherent neutron scattering length value, 8.9(1) fm, is reported.

cond-mat.str-el↗

arXiv2015

The Valence-Fluctuating Ground State of Plutonium

A central issue in material science is to obtain understanding of the electronic correlations that control complex materials. Such electronic correlations frequently arise due to the competition of localized and itinerant electronic degrees of freedom. While the respective limits of well-localized or entirely itinerant ground states are well-understood, the intermediate regime that controls the functional properties of complex materials continues to challenge theoretical understanding. We have used neutron spectroscopy to investigate plutonium, which is a prototypical material at the brink between bonding and non-bonding configurations. Our study reveals that the ground state of plutonium is governed by valence fluctuations, that is, a quantum-mechanical superposition of localized and itinerant electronic configurations as recently predicted by dynamical mean field theory. Our results not only resolve the long-standing controversy between experiment and theory on plutonium's magnetism, but also suggest an improved understanding of the effects of such electronic dichotomy in complex materials.

cond-mat.str-el↗

arXiv2015

Emergent excitation at the magnetic metal-insulator transition in the pyrochlore osmate Cd2Os2O7

The rich physics manifested by 5d oxides falls outside the Mott-Hubbard paradigm used to successfully explain the electronic and magnetic properties of 3d oxides. Much consideration has been given to the extent to which strong spin-orbit coupling (SOC), in the limit of increased bandwidth and reduced electron correlation, drives the formation of novel electronic states, as manifested through the existence of metal-insulator transitions (MITs). SOC is believed to play a dominant role in 5d5 systems such as iridates (Ir4+), undergoing MITs which may or may not be intimately connected to magnetic order, with pyrochlore and perovksite systems being examples of the former and latter, respectively. However, the role of SOC for other 5d configurations is less clear. For example, 5d3 (e.g Os5+) systems are expected to have an orbital singlet and consequently a reduced effect of SOC in the groundstate. The pyrochlore osmate Cd2Os2O7 nonetheless exhibits a MIT intimately entwined with magnetic order with phenomena similar to pyrochlore iridates. Here we report the first resonant inelastic X-ray scattering (RIXS) measurements on an osmium compound, allowing us to determine the salient electronic and magnetic energy scales controlling the MIT in Cd2Os2O7, which we benchmark against detailed quantum chemistry calculations. In particular, we reveal the emergence at the MIT of a magnetic excitation corresponding to a superposition of multiple spin-flip processes from an Ising-like all-in/all-out magnetic groundstate. We discuss our results with respect to the role of SOC in magnetically mediated MITs in 5d systems

cond-mat.str-el↗

arXiv2015

Evolution of competing magnetic order in the Jeff=1/2 insulating state of Sr2Ir1-xRuxO4

We investigate the magnetic properties of the series Sr2Ir1-xRuxO4 with neutron, resonant x-ray and magnetization measurements. The results indicate an evolution and coexistence of magnetic structures via a spin flop transition from ab-plane to c-axis collinear order as the 5d Ir4+ ions are replaced with an increasing concentration of 4d Ru4+ ions. The magnetic structures within the ordered regime of the phase diagram (x<0.3) are reported. Despite the changes in magnetic structure no alteration of the Jeff=1/2 ground state is observed. The behavior of Sr2Ir1-xRuxO4 is consistent with electronic phase separation and diverges from a standard scenario of hole doping. The role of lattice alterations with doping on the magnetic and insulating behavior is considered. The results presented here provide insight into the magnetic insulating states in strong spin-orbit coupled materials and the role perturbations play in altering the behavior.

cond-mat.str-el↗

arXiv2015

Magnetic Correlations in the Quasi-2D Semiconducting Ferromagnet CrSiTe$_3$

Intrinsic, two-dimensional ferromagnetic semiconductors are an important class of materials for overcoming the limitations of dilute magnetic semiconductors for spintronics applications. CrSiTe$_3$ is a particularly interesting member of this class, since it can likely be exfoliated down to single layers, where T$_C$ is predicted to increase dramatically. Establishing the nature of the magnetism in the bulk is a necessary precursor to understanding the magnetic behavior in thin film samples and the possible applications of this material. In this work, we use elastic and inelastic neutron scattering to measure the magnetic properties of single crystalline CrSiTe$_3$. We find that there is a very small single ion anisotropy favoring magnetic ordering along the $c$-axis and that the measured spin waves fit well to a model where the moments are only weakly coupled along that direction. Finally, we find that both static and dynamic correlations persist within the $ab$-plane up to at least 300 K, strong evidence of this material's two-dimensional characteristics that are relevant for future studies on thin film and monolayer samples.

cond-mat.str-el↗

arXiv2015

Influence of interstitial Mn on magnetism in room-temperature ferromagnet Mn(1+delta)Sb

We report elastic and inelastic neutron scattering measurements of the high-TC ferromagnet Mn(1+delta)Sb. Measurements were performed on a large, TC=434 K, single crystal with interstitial Mn content of delta~0.13. The neutron diffraction results reveal that the interstitial Mn has a magnetic moment, and that it is aligned antiparallel to the main Mn moment. We perform density functional theory calculations including the interstitial Mn, and find the interstitial to be magnetic in agreement with the diffraction data. The inelastic neutron scattering measurements reveal two features in the magnetic dynamics: i) a spin-wave-like dispersion emanating from ferromagnetic Bragg positions (H K 2n), and ii) a broad, non-dispersive signal centered at forbidden Bragg positions (H$\,$K$\,$2$n$+1). The inelastic spectrum cannot be modeled by simple linear spin-wave theory calculations, and appears to be significantly altered by the presence of the interstitial Mn ions. The results show that the influence of the interstitial Mn on the magnetic state in this system is more important than previously understood.

cond-mat.str-el↗

arXiv2015

Proximate Kitaev Quantum Spin Liquid Behaviour in α-RuCl$_3$

Topological states of matter such as quantum spin liquids (QSLs) are of great interest because of their remarkable predicted properties including protection of quantum information and the emergence of Majorana fermions. Such QSLs, however, have proven difficult to identify experimentally. The most promising approach is to study their exotic nature via the wave-vector and intensity dependence of their dynamical response in neutron scattering. A major search has centered on iridate materials which are proposed to realize the celebrated Kitaev model on a honeycomb lattice - a prototypical topological QSL system in two dimensions (2D). The difficulties of iridium for neutron measurements have, however, impeded progress significantly. Here we provide experimental evidence that a material based on ruthenium, α-RuCl$_3$ realizes the same Kitaev physics but is highly amenable to neutron investigation. Our measurements confirm the requisite strong spin-orbit coupling, and a low temperature magnetic order that matches the predicted phase proximate to the QSL. We also show that stacking faults, inherent to the highly 2D nature of the material, readily explain some puzzling results to date. Measurements of the dynamical response functions, especially at energies and temperatures above that where interlayer effects are manifest, are naturally accounted for in terms of deconfinement physics expected for QSLs. Via a comparison to the recently calculated dynamics from gauge flux excitations and Majorana fermions of the pure Kitaev model we propose α-RuCl$_3$ as the prime candidate for experimental realization of fractionalized Kitaev physics.

cond-mat.mtrl-sci↗

arXiv2015

Magnetic order and electronic structure of 5d3 double perovskite Sr2ScOsO6

The magnetic susceptibility, crystal and magnetic structures, and electronic structure of double perovskite Sr2ScOsO6 are reported. Using both neutron and x-ray powder diffraction we find that the crystal structure is monoclinic P21/n from 3.5 to 300 K. Magnetization measurements indicate an antiferromagnetic transition at TN=92K, one of the highest transition temperatures of any double perovskite hosting only one magnetic ion. Type I antiferromagnetic order is determined by neutron powder diffraction, with an Os moment of only 1.6(1) muB, close to half the spin-only value for a crystal field split 5d electron state with t2g^3 ground state. Density functional calculations show that this reduction is largely the result of strong Os-O hybridization, with spin-orbit coupling responsible for only a ~0.1 muB reduction in the moment.

cond-mat.str-el↗

arXiv2015

Interaction Driven Subgap Spin Exciton in the Kondo Insulator SmB6

Using inelastic neutron scattering, we map a 14 meV coherent resonant mode in the topological Kondo insulator SmB6 and describe its relation to the low energy insulating band structure. The resonant intensity is confined to the X and R high symmetry points, repeating outside the first Brillouin zone and dispersing less than 2 meV, with a 5d-like magnetic form factor. We present a slave-boson treatment of the Anderson Hamiltonian with a third neighbor dominated hybridized band structure. This approach produces a spin exciton below the charge gap with features that are consistent with the observed neutron scattering. We find that maxima in the wave vector dependence of the inelastic neutron scattering indicate band inversion.

cond-mat.str-el↗

arXiv2015

Giant spin-phonon-electronic coupling in a 5d oxide

Enhanced coupling of material properties offers new fundamental insights and routes to multifunctional devices. In this context 5d oxides provide new paradigms of cooperative interactions driving novel emergent behavior. This is exemplified in 5d osmates that host a metal-insulator transition (MIT) driven by magnetic order. Here we consider the most robust case, the 5d perovskite NaOsO3, and reveal a giant coupling between spin and phonon through a frequency shift of Δω=40 cm-1, the largest measured in any material. We identify the dominant octahedral breathing mode and show isosymmetry with spin ordering which induces dynamic charge disproportionation that sheds new light on the MIT. The occurrence of the dramatic spin-phonon-electronic coupling in NaOsO3 is due to a property common to all 5d materials: the large spatial extent of the 5d ion. This allows magnetism to couple to phonons on an unprecedented scale and consequently offers multiple new routes to enhanced coupled phenomena.

cond-mat.str-el↗

arXiv2014

Anisotropic inplane spin correlation in the parent and Co-doped BaFe2As2: a neutron scattering study

Antiferromagnetic spin fluctuations were investigated in the normal states of the parent ($x = 0$), under-doped ($x = 0.04$) and optimally-doped ($x = 0.06$) Ba(Fe$_{1-x}$Co$_x$)$_2$As$_2$ single crystals using inelastic neutron scattering technique. For all the doping levels, quasi-two-dimensional antiferromagnetic fluctuations were observed as a broad peak localized at ${\it Q} = (1/2, 1/2, l)$. At lower energies, the peak shows an apparent anisotropy in the $hk0$ plane; longitudinal peak widths are considerably smaller than transverse widths. The anisotropy is larger for the higher doping level. These results are consistent with the random phase approximation (RPA) calculations taking account of the orbital character of the electronic bands, confirming that the anisotropic nature of the spin fluctuations in the normal states is mostly dominated by the nesting of Fermi surfaces. On the other hand, the quasi-two-dimensional spin correlations grow much rapidly for decreasing temperature in the $x = 0$ parent compound, compared to that expected for nearly antiferromagnetic metals. This may be another sign of the unconventional nature of the antiferromagnetic transition in BaFe$_2$As$_2$.

cond-mat.supr-con↗

arXiv2014

Crossover from spin-waves to diffusive spin excitations in underdoped Ba(Fe$_{1-x}$Co$_{x}$)$_{2}$As$_{2}$

Using inelastic neutron scattering, we show that the onset of superconductivity in underdoped Ba(Fe$_{1-x}$Co$_{x}$)$_{2}$As$_{2}$ coincides with a crossover from well-defined spin waves to overdamped and diffusive spin excitations. This crossover occurs despite the presence of long-range stripe antiferromagnetic order for samples in a compositional range from x=0.04-0.055, and is a consequence of the shrinking spin-density wave gap and a corresponding increase in the particle-hole (Landau) damping. The latter effect is captured by a simple itinerant model relating Co doping to changes in the hot spots of the Fermi surface. We argue that the overdamped spin fluctuations provide a pairing mechanism for superconductivity in these materials.

cond-mat.supr-con↗

arXiv2014

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.

cond-mat.str-el↗

arXiv2013

Magnetic structure and spin excitations in BaMn2Bi2

We present a single crystal neutron scattering study of BaMn2Bi2, a recently synthesized material with the same ThCr2Si2-type structure found in several Fe-based unconventional superconducting materials. We show long range magnetic order, in the form of a G-type antiferromagnetic structure, to exist up to 390 K with an indication of a structural transition at 100 K. Utilizing inelastic neutron scattering we observe a spin-gap of 16meV, with spin-waves extending up to 55 meV. We find these magnetic excitations to be well fit to a J1-J2-Jc Heisenberg model and present values for the exchange interactions. The spin wave spectrum appears to be unchanged by the 100 K structural phase transition.

cond-mat.str-el↗