arXiv subjects

A. D. Christianson

Publications and source records attributed to A. D. Christianson.

At least 55 records · Page 3Linked to original sources

arXiv2016

Strong anisotropy within a Heisenberg model in the J=1/2 insulating state of Sr2Ir0.8Ru0.2O4

The dispersive magnetic excitations in Sr2IrO4 have previously been well described within an isospin-1/2 Heisenberg model on a square lattice that revealed parallels with La2CuO4. Here we investigate the inelastic spectra of Sr2Ir0.8Ru0.2O4 with resonant inelastic x-ray scattering (RIXS) at the Ir L3-edge. The results are well described using linear spin-wave theory within a similar Heisenberg model applicable to Sr2IrO4, however the disorder induced by the substitution of 20% Ir4+ ions for Ru4+ removes longer range exchange interactions. A large spin-gap (40 meV) is measured indicating strong anisotropy from spin-orbit coupling that is manifest due to the altered magnetic structure in Sr2Ir0.8Ru0.2O4 with c-axis aligned moments compared to the basal plane moments in the parent. Collectively the results indicate the robustness of a Heisenberg model description even when the magnetic structure is altered and the J=1/2 moments diluted.

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arXiv2016

Spin-orbit coupling controlled $J=3/2$ electronic ground state in 5$d^{3}$ oxides

Entanglement of spin and orbital degrees of freedom drives the formation of novel quantum and topological physical states. Discovering new spin-orbit entangled ground states and emergent phases of matter requires both experimentally probing the relevant energy scales and applying suitable theoretical models. Here we report resonant inelastic x-ray scattering measurements of the transition metal oxides Ca$_3$LiOsO$_6$ and Ba$_2$YOsO$_6$. We invoke an intermediate coupling approach that incorporates both spin-orbit coupling and electron-electron interactions on an even footing and reveal the ground state of $5d^3$ based compounds, which has remained elusive in previously applied models, is a novel spin-orbit entangled J=3/2 electronic ground state. This work reveals the hidden diversity of spin-orbit controlled ground states in 5d systems and introduces a new arena in the search for spin-orbit controlled phases of matter.

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arXiv2016

Strong ferromagnetic exchange interaction in the parent state of the superconductivity in BaFe$_2$S$_3$

Inelastic neutron scattering measurements have been performed to investigate the spin waves of the quasi-one-dimensional antiferromagnetic ladder compound BaFe$_2$S$_3$, where a superconducting transition was observed under pressure [H. Takahashi {\it et al.}, Nat. Mater. 14, 1008-1012 (2015); T. Yamauchi {\it et al.}, Phys. Rev. Lett. 115, 246402 (2015)]. By fitting the spherically averaged experimental data collected on a powder sample to a Heisenberg Hamiltonian, we find that the one-dimensional antiferromagnetic ladder exhibits a strong nearest neighbor ferromagnetic exchange interaction ($SJ_R=-71\pm4$ meV) along the rung direction, an antiferromagnetic $SJ_L=49\pm3$ meV along the leg direction and a ferromagnetic $SJ_2=-15\pm2$ meV along the diagonal direction. Our data demonstrate that the antiferromagnetic spin excitations are a common characteristic for the iron-based superconductors, while specific relative values for the exchange interactions do not appear to be unique for the parent states of the superconducting materials.

cond-mat.supr-con↗

arXiv2016

Candidate Elastic Quantum Critical Point in LaCu$_{6-x}$Au$_x$

The structural properties of LaCu$_{6-x}$Au$_x$ have been studied using neutron diffraction, x-ray diffraction, and heat capacity measurements. The continuous orthorhombic-monoclinic structural phase transition in LaCu$_{6}$ is suppressed linearly with Au substitution until a complete suppression of the structural phase transition occurs at the critical composition, $x_{c}$ = 0.3. Heat capacity measurements at low temperatures indicate residual structural instability at $x_c$ that extends well into the orthorhombic phase. The instability is ferroelastic in nature, with density functional theory (DFT) calculations showing negligible coupling to electronic states near the Fermi level. The data and calculations presented here are consistent with the zero temperature termination of a continuous structural phase transition suggesting that the LaCu$_{6-x}$Au$_x$ series hosts an elastic quantum critical point.

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arXiv2016

Magnetic ground state of FeSe

Elucidating the nature of the magnetism of a high-temperature superconductor is crucial for establishing its pairing mechanism. The parent compounds of the cuprate and iron-pnictide superconductors exhibit Néel and stripe magnetic order, respectively. However, FeSe, the structurally simplest iron-based superconductor, shows nematic order (Ts = 90 K), but not magnetic order in the parent phase, and its magnetic ground state is intensely debated. Here, we report inelastic neutron-scattering experiments that reveal both stripe and Néel spin fluctuations over a wide energy range at 110 K. On entering the nematic phase, a substantial amount of spectral weight is transferred from the Néel to the stripe spin fluctuations. Moreover, the total fluctuating magnetic moment of FeSe is ~ 60% larger than that in the iron pnictide BaFe2As2. Our results suggest that FeSe is a novel S = 1 nematic quantum-disordered paramagnet interpolating between the Néel and stripe magnetic instabilities.

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arXiv2016

Spin waves and magnetic exchange interactions in the spin ladder compound RbFe$_2$Se$_3$

We report an inelastic neutron scattering study of the spin waves of the one-dimensional antiferromagnetic spin ladder compound RbFe$_2$Se$_3$. The results reveal that the products, $SJ$'s, of the spin $S$ and the magnetic exchange interactions $J$'s along the antiferromagnetic (leg) direction and the ferromagnetic (rung) direction are comparable with those for the stripe ordered phase of the parent compounds of the iron-based superconductors. The universality of the $SJ$'s implies nearly universal spin wave dynamics and the irrelevance of the fermiology for the existence of the stripe antiferromagnetic order among various Fe-based materials.

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arXiv2016

Spin-orbit coupling control of anisotropy, ground state and frustration in 5d2 Sr2MgOsO6

The influence of spin-orbit coupling (SOC) on the physical properties of the 5d2 system Sr2MgOsO6 is probed via a combination of magnetometry, specific heat measurements, elastic and inelastic neutron scattering, and density functional theory calculations. Although a significant degree of frustration is expected, we find that Sr2MgOsO6 orders in a type I antiferromagnetic structure at the remarkably high temperature of 108 K. The measurements presented allow for the first accurate quantification of the size of the magnetic moment in a 5d2 system of 0.60(2) muB - a significantly reduced moment from the expected value for such a system. Furthermore, significant anisotropy is identified via a spin excitation gap, and we confirm by first principles calculations that SOC not only provides the magnetocrystalline anisotropy, but also plays a crucial role in determining both the ground state magnetic order and the size of the local moment in this compound. Through comparison to Sr2ScOsO6, it is demonstrated that SOC-induced anisotropy has the ability to relieve frustration in 5d2 systems relative to their 5d3 counterparts, providing an explanation of the high TN found in Sr2MgOsO6.

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arXiv2016

Electron doping evolution of the neutron spin resonance in NaFe$_{1-x}$Co$_{x}$As

Neutron spin resonance, a collective magnetic excitation coupled to superconductivity, is one of the most prominent features shared by a broad family of unconventional superconductors including copper oxides, iron pnictides, and heavy fermions. In this work, we study the doping evolution of the resonances in NaFe$_{1-x}$Co$_x$As covering the entire superconducting dome. For the underdoped compositions, two resonance modes coexist. As doping increases, the low-energy resonance gradually loses its spectral weight to the high-energy one but remains at the same energy. By contrast, in the overdoped regime we only find one single resonance, which acquires a broader width in both energy and momentum, but retains approximately the same peak position even when $T_c$ drops by nearly a half compared to optimal doping. These results suggest that the energy of the resonance in electron overdoped NaFe$_{1-x}$Co$_x$As is neither simply proportional to $T_c$ nor the superconducting gap, but is controlled by the multi-orbital character of the system and doped impurity scattering effect.

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arXiv2016

Experimental elucidation of the origin of the `double spin resonances' in Ba(Fe$_{1-x}$Co$_x$)$_2$As$_2$

We report a combined study of the spin resonances and superconducting gaps for underdoped ($T_c=19$ K), optimally doped ($T_c=25$ K), and overdoped ($T_c=19$ K) Ba(Fe$_{1-x}$Co$_x$)$_2$As$_2$ single crystals with inelastic neutron scattering and angle resolved photoemission spectroscopy. We find a quasi two dimensional spin resonance whose energy scales with the superconducting gap in all three compounds. In addition, anisotropic low energy spin excitation enhancements in the superconducting state have been deduced and characterized for the under and optimally doped compounds. Our data suggest that the quasi two dimensional spin resonance is a spin exciton that corresponds to the spin singlet-triplet excitations of the itinerant electrons. However, the intensity enhancements of the anisotropic spin excitations are dominated by the out-of-plane spin excitations of the ordered moments due to the suppression of damping in the superconducting state. Hence we offer a new interpretation of the double energy scales differing from previous interpretations based on anisotropic superconducting energy gaps, and systematically explain the doping-dependent trend across the phase diagram.

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arXiv2016

Dominant Kitaev interactions on the fcc lattice in iridate double perovskites La2BIrO6 (B=Mg, Zn)

We have performed inelastic neutron scattering experiments to investigate the magnetic excitations in the quasi-face-centered-cubic (fcc) iridate double perovskites La2ZnIrO6 and La2MgIrO6, which are characterized by A-type antiferromagnetic ground states. The neutron scattering data, which reveal gapped spin wave excitations with a very weak dispersion, are shown to be well-described by theoretical calculations on a model Hamiltonian with dominant Kitaev interactions. Our surprising finding shows that in contrast to honeycomb materials, where the Kitaev interaction manifests itself via complex magnetic order, even conventional magnetic orders in certain geometrically frustrated systems might owe their existence to unconventional Kitaev exchange.

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arXiv2016

Highly-anisotropic exchange interactions of $j_{\rm eff}=1/2$ iridium moments on the fcc lattice in La$_2B$IrO$_6$ ($B$ $=$ Mg, Zn)

We have performed inelastic neutron scattering (INS) experiments to investigate the magnetic excitations in the weakly distorted face-centered-cubic (fcc) iridate double perovskites La$_2$ZnIrO$_6$ and La$_2$MgIrO$_6$, which are characterized by A-type antiferromagnetic ground states. The powder inelastic neutron scattering data on these geometrically frustrated $j_{\rm eff}=1/2$ Mott insulators provide clear evidence for gapped spin wave excitations with very weak dispersion. The INS results and thermodynamic data on these materials can be reproduced by conventional Heisenberg-Ising models with significant uniaxial Ising anisotropy and sizeable second-neighbor ferromagnetic interactions. Such a uniaxial Ising exchange interaction is symmetry-forbidden on the ideal fcc lattice, so that it can only arise from the weak crystal distortions away from the ideal fcc limit. This may suggest that even weak distortions in $j_{\rm eff}=1/2$ Mott insulators might lead to strong exchange anisotropies. More tantalizingly, however, we find an alternative viable explanation of the INS results in terms of spin models with a dominant Kitaev interaction. In contrast to the uniaxial Ising exchange, the highly-directional Kitaev interaction is a type of exchange anisotropy which is symmetry-allowed even on the ideal fcc lattice. The Kitaev model has a magnon gap induced by quantum order-by-disorder, while weak anisotropies of the Kitaev couplings generated by the symmetry-lowering due to lattice distortions, can pin the order and enhance the magnon gap. Our findings highlight how even conventional magnetic orders in heavy transition metal oxides may be driven by highly-directional exchange interactions rooted in strong spin-orbit coupling.

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arXiv2016

Spin-orbit coupling controlled ground state in Sr$_2$ScOsO$_6$

We report neutron scattering experiments which reveal a large spin gap in the magnetic excitation spectrum of weakly-monoclinic double perovskite Sr2ScOsO6. The spin gap is demonstrative of appreciable spin-orbit-induced anisotropy, despite nominally orbitally-quenched 5d3 Os5+ ions. The system is successfully modeled including nearest neighbor interactions in a Heisenberg Hamiltonian with exchange anisotropy. We find that the presence of the spin-orbit-induced anisotropy is essential for the realization of the type I antiferromagnetic ground state. This demonstrates that physics beyond the LS or JJ coupling limits plays an active role in determining the collective properties of 4d3 and 5d3 systems, and that theoretical treatments must include spin-orbit coupling.

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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.

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arXiv2016

Commensurate antiferromagnetic excitations as a signature of the pseudogap in the tetragonal high-Tc cuprate HgBa$_2$CuO$_{4+δ}$

Antiferromagnetic correlations have been argued to be the cause of the d-wave superconductivity and the pseudogap phenomena exhibited by the cuprates. Although the antiferromagnetic response in the pseudogap state has been reported for a number of compounds, there exists no information for structurally simple HgBa$_2$CuO$_{4+δ}$. Here we report neutron scattering results for HgBa$_2$CuO$_{4+δ}$ (superconducting transition temperature T$_c$ $\sim$ 71 K, pseudogap temperature T* $\sim$ 305 K) that demonstrate the absence of the two most prominent features of the magnetic excitation spectrum of the cuprates: the X-shaped 'hourglass' response and the resonance mode in the superconducting state. Instead, the response is Y-shaped, gapped, and significantly enhanced below T*, and hence a prominent signature of the pseudogap state.

cond-mat.supr-con↗

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.

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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.

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arXiv2015

Spin dynamics near a putative antiferromagnetic quantum critical point in Cu substituted BaFe$_2$As$_2$ and its relation to high-temperature superconductivity

We present the results of elastic and inelastic neutron scattering measurements on non-superconducting Ba(Fe${_{0.957}}$Cu${_{0.043}}$)${_2}$As${_2}$, a composition close to a quantum critical point between AFM ordered and paramagnetic phases. By comparing these results with the spin fluctuations in the low Cu composition as well as the parent compound BaFe$_2$As$_2$ and superconducting Ba(Fe$_{1-x}$Ni$_x$)$_2$As$_2$ compounds, we demonstrate that paramagnon-like spin fluctuations are evident in the antiferromagnetically ordered state of Ba(Fe$_{0.957}$Cu$_{0.043}$)$_2$As$_2$, which is distinct from the AFM-like spin fluctuations in the superconducting compounds. Our observations suggest that Cu substitution decouples the interaction between quasiparticles and the spin fluctuations. We also show that the spin-spin correlation length, ${ξ(T)}$, increases rapidly as the temperature is lowered and find ${ω/T}$ scaling behavior, the hallmark of quantum criticality, at an antiferromagnetic quantum critical point.

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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

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