arXiv subjects

D. F. McMorrow

Publications and source records attributed to D. F. McMorrow.

At least 19 recordsLinked to original sources

arXiv2024

Spin dynamics and possible topological magnons in non-stoichiometric pyrochlore iridate Tb$_2$Ir$_2$O$_7$ studied by RIXS

We report a resonant inelastic X-ray scattering study on a single crystal of a non-stoichiometric pyrochlore iridate Tb$_{2+x}$Ir$_{2-x}$O$_{7-y}$ ($x \simeq 0.25$) that magnetically orders at $T_{\rm{N}}\simeq 50$ K. We find that the strength of the spin-orbit coupling and the trigonal distortion of the IrO$_6$ octahedra are comparable with the ones obtained in other pyrochlore iridates. We observe a propagating gapped magnon mode at low energy, and model it using a Hamiltonian consisting of a Heisenberg exchange [$J = 16.2(9)$ meV] and Dzyaloshinskii-Moriya interactions [$D = 5.2(3)$ meV], which shows the robustness of interactions despite Tb-stuffing at the Ir-site. Strikingly, the ratio $D/J = 0.32(3)$ supports possible non-trivial topological magnon band crossing. This material may thus host coexisting fermionic and bosonic topology, with potential for manipulating electronic and magnonic topological bands thanks to the $d-f$ interaction.

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arXiv2023

Strain control of a bandwidth-driven spin reorientation in Ca$_{3}$Ru$_{2}$O$_{7}$

The layered-ruthenate family of materials possess an intricate interplay of structural, electronic and magnetic degrees of freedom that yields a plethora of delicately balanced ground states. This is exemplified by Ca$_{3}$Ru$_{2}$O$_{7}$, which hosts a coupled transition in which the lattice parameters jump, the Fermi surface partially gaps and the spins undergo a $90^{\circ}$ in-plane reorientation. Here, we show how the transition is driven by a lattice strain that tunes the electronic bandwidth. We apply uniaxial stress to single crystals of Ca$_{3}$Ru$_{2}$O$_{7}$, using neutron and resonant x-ray scattering to simultaneously probe the structural and magnetic responses. These measurements demonstrate that the transition can be driven by externally induced strain, stimulating the development of a theoretical model in which an internal strain is generated self-consistently to lower the electronic energy. We understand the strain to act by modifying tilts and rotations of the RuO$_{6}$ octahedra, which directly influences the nearest-neighbour hopping. Our results offer a blueprint for uncovering the driving force behind coupled phase transitions, as well as a route to controlling them.

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arXiv2022

The magnetic structure and field dependence of the cycloid phase mediating the spin reorientation transition in Ca$_3$Ru$_2$O$_7$

We report a comprehensive experimental investigation of the magnetic structure of the cycloidal phase in Ca$_3$Ru$_2$O$_7$, which mediates the spin reorientation transition, and establishes its magnetic phase diagram. In zero applied field, single-crystal neutron diffraction data confirms the scenario deduced from an earlier resonant x-ray scattering study: between $46.7$~K $< T < 49.0$~K the magnetic moments form a cycloid in the $a-b$ plane with a propagation wavevector of $(δ,0,1)$ with $δ\simeq 0.025$ and an ordered moment of about 1 $μ_{\rm{B}}$, with the eccentricity of the cycloid evolving with temperature. In an applied magnetic field applied parallel to the $b$-axis, the intensity of the $(δ,0,1)$ satellite peaks decreases continuously up to about $μ_0 H \simeq 5$ T, above which field the system becomes field polarised. Both the eccentricity of the cycloid and the wavevector increase with field, the latter suggesting an enhancement of the anti$-$symmetric Dzyaloshinskii$-$Moriya interaction via magnetostriction effects. Transitions between the various low-temperature magnetic phases have been carefully mapped out using magnetometry and resistivity. The resulting phase diagram reveals that the cycloid phase exists in a temperature window that expands rapidly with increasing field, before transitioning to a polarised paramagnetic state at 5 T. High-field magnetoresistance measurements show that below $T\simeq 70$ K the resistivity increases continuously with decreasing temperature, indicating the inherent insulating nature at low temperatures of our high-quality, untwinned, single-crystals. We discuss our results with reference to previous reports of the magnetic phase diagram of Ca$_3$Ru$_2$O$_7$ that utilised samples which were more metallic and/or poly-domain.

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arXiv2022

Probing electron-phonon interactions away from the Fermi level with resonant inelastic x-ray scattering

Interactions between electrons and lattice vibrations are responsible for a wide range of material properties and applications. Recently, there has been considerable interest in the development of resonant inelastic x-ray scattering (RIXS) as a tool for measuring electron-phonon (e-ph) interactions. Here, we demonstrate the ability of RIXS to probe the interaction between phonons and specific electronic states both near to, and away from, the Fermi level. We performed carbon $K$-edge RIXS measurements on graphite, tuning the incident x-ray energy to separately probe the interactions of the $π^*$ and $σ^*$ electronic states. Our high-resolution data reveals detailed structure in the multi-phonon RIXS features that directly encodes the momentum dependence of the e-ph interaction strength. We develop a Green's-function method to model this structure, which naturally accounts for the phonon and interaction-strength dispersions, as well as the mixing of phonon momenta in the intermediate state. This model shows that the differences between the spectra can be fully explained by contrasting trends of the e-ph interaction through the Brillouin zone, being concentrated at the $Γ$ and $K$ points for the $π^*$ states, while being significant at all momenta for the $σ^*$ states. Our results advance the interpretation of phonon excitations in RIXS, and extend its applicability as a probe of e-ph interactions to a new range of out-of-equilibrium situations.

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arXiv2021

Laser-Induced Transient Magnons in Sr3Ir2O7 Throughout the Brillouin Zone

Although ultrafast manipulation of magnetism holds great promise for new physical phenomena and applications, targeting specific states is held back by our limited understanding of how magnetic correlations evolve on ultrafast timescales. Using ultrafast resonant inelastic x-ray scattering we demonstrate that femtosecond laser pulses can excite transient magnons at large wavevectors in gapped antiferromagnets, and that they persist for several picoseconds which is opposite to what is observed in nearly gapless magnets. Our work suggests that materials with isotropic magnetic interactions are preferred to achieve rapid manipulation of magnetism.

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arXiv2020

Spontaneous cycloidal order mediating a spin-reorientation transition in a polar metal

We show how complex modulated order can spontaneously emerge when magnetic interactions compete in a metal with polar lattice distortions. Combining neutron and resonant x-ray scattering with symmetry analysis, we reveal that the spin reorientation in Ca$_3$Ru$_2$O$_7$ is mediated by a magnetic cycloid whose eccentricity evolves smoothly but rapidly with temperature. We find the cycloid to be highly sensitive to magnetic fields, which appear to continuously generate higher harmonic modulations. Our results provide a unified picture of the rich magnetic phases of this correlated, multi-band polar metal.

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arXiv2020

Correlated electron metal properties of the honeycomb ruthenate Na$_2$RuO$_3$

We report the synthesis and characterisation of polycrystalline Na$_2$RuO$_3$, a layered material in which the Ru$^{4+}$ ($4d^4$ configuration) form a honeycomb lattice. The optimal synthesis condition was found to produce a nearly ordered Na$_2$RuO$_3$ ($C2/c$ phase), as assessed from the refinement of the time-of-flight neutron powder diffraction. Magnetic susceptibility measurements reveal a large temperature-independent Pauli paramagnetism ($χ_0 \sim 1.42(2)\times10^{-3}$ emu/mol Oe) with no evidence of magnetic ordering down to 1.5 K, and with an absence of dynamic magnetic correlations, as evidenced by neutron scattering spectroscopy. The intrinsic susceptibility ($χ_0$) together with the Sommerfeld coeficient of $γ=11.7(2)$ mJ/Ru mol K$^2$ estimated from heat capacity measurements, gives an enhanced Wilson ratio of $R_W\approx8.9(1)$, suggesting that magnetic correlations may be present in this material. While transport measurements on pressed pellets show nonmetallic behaviour, photoemission spectrocopy indicate a small but finite density of states at the Fermi energy, suggesting that the bulk material is metallic. Except for resistivity measurements, which may have been compromised by near surface and interface effects, all other probes indicate that Na$_2$RuO$_3$ is a moderately correlated electron metal. Our results thus stand in contrast to earlier reports that Na$_2$RuO$_3$ is an antiferromagnetic insulator at low temperatures.

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arXiv2020

Thermal control of spin excitations in the coupled Ising-chain material RbCoCl3

We have used neutron spectroscopy to investigate the spin dynamics of the quantum (S = 1/2) antiferromagnetic Ising chains in RbCoCl3. The structure and magnetic interactions in this material conspire to produce two magnetic phase transitions at low temperatures, presenting an ideal opportunity for thermal control of the chain environment. The high-resolution spectra we measure of two-domain-wall excitations therefore characterize precisely both the continuum response of isolated chains and the "Zeeman-ladder" bound states of chains in three different effective staggered fields in one and the same material. We apply an extended Matsubara formalism to obtain a quantitative description of the entire dataset, Monte Carlo simulations to interpret the magnetic order, and finite-temperature DMRG calculations to fit the spectral features of all three phases.

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arXiv2020

Spin and orbital dynamics through the metal-to-insulator transition in Cd$_2$Os$_2$O$_7$ probed with high-resolution RIXS

High-resolution resonant inelastic x-ray scattering (RIXS) measurements ($Δ$E = 46 meV) have been performed on Cd$_2$Os$_2$O$_7$ through the metal-to-insulator transition (MIT). A magnetic excitation at 125 meV evolves continuously through the MIT, in agreement with recent Raman scattering results, and provides further confirmation for an all-in, all-out magnetic ground state. Asymmetry of this feature is likely a result of coupling between the electronic and magnetic degrees of freedom. We also observe a broad continuum of interband excitations centered at 0.3 eV energy loss. This is indicative of significant hybridization between Os 5$d$ and O 2$p$ states, and concurrent itinerant nature of the system. In turn, this suggests a possible break down of the free-ion model for Cd$_2$Os$_2$O$_7$.

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arXiv2019

Temperature dependence of the $(π,0)$ anomaly in the excitation spectrum of the 2D quantum Heisenberg antiferromagnet

It is well established that in the low-temperature limit, the two-dimensional quantum Heisenberg antiferromagnet on a square lattice (2DQHAFSL) exhibits an anomaly in its spectrum at short-wavelengths on the zone-boundary. In the vicinity of the $(π,0)$ point the pole in the one-magnon response exhibits a downward dispersion, is heavily damped and attenuated, giving way to an isotropic continuum of excitations extending to high energies. The origin of the anomaly and the presence of the continuum are of current theoretical interest, with suggestions focused around the idea that the latter evidences the existence of spinons in a two-dimensional system. Here we present the results of neutron inelastic scattering experiments and Quantum Monte Carlo calculations on the metallo-organic compound Cu(DCOO)$_2\cdot 4$D$_2$O (CFTD), an excellent physical realisation of the 2DQHAFSL, designed to investigate how the anomaly at $(π,0)$ evolves up to finite temperatures $T/J\sim2/3$. Our data reveal that on warming the anomaly survives the loss of long-range, three-dimensional order, and is thus a robust feature of the two-dimensional system. With further increase of temperature the zone-boundary response gradually softens and broadens, washing out the $(π,0)$ anomaly. This is confirmed by a comparison of our data with the results of finite-temperature Quantum Monte Carlo simulations where the two are found to be in good accord. At lower energies, in the vicinity of the antiferromagnetic zone centre, there was no significant softening of the magnetic excitations over the range of temperatures investigated.

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arXiv2019

High-resolution resonant inelastic x-ray scattering study of the electron-phonon coupling in honeycomb $α$-Li$_2$IrO$_3$

The excitations in honeycomb $α$-Li$_2$IrO$_3$ have been investigated with high-resolution resonant inelastic x-ray scattering (RIXS) at the O K edge. The low-energy response is dominated by a fully resolved ladder of excitations, which we interpret as being due to multi-phonon processes in the presence of strong electron-phonon coupling (EPC). At higher energies, the orbital excitations are shown to be dressed by phonons. The high quality of the data permits a quantitative test of the analytical model for the RIXS cross-section, which has been proposed to describe EPC in transition metal oxides (TMOs). We find that the magnitude of the EPC is comparable to that found for a range of 3d TMOs. This indicates that EPC may be of equal importance in determining the phenomenology displayed by corresponding 5d based systems.

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arXiv2019

Selective probing of magnetic order on Tb and Ir sites in stuffed Tb$_{2+x}$Ir$_{2-x}$O$_{7-y}$ using resonant X-ray scattering

We study the magnetic structure of the "stuffed" (Tb-rich) pyrochlore iridate Tb$_{2+x}$Ir$_{2-x}$O$_{7-y}$, using resonant elastic x-ray scattering (REXS). In order to disentangle contributions from Tb and Ir magnetic sublattices, experiments were performed at the Ir $L_3$ and Tb $M_5$ edges, which provide selective sensitivity to Ir $5d$ and Tb $4f$ magnetic moments, respectively. At the Ir $L_3$ edge, we found the onset of long-range ${\bf k}={\bf 0}$ magnetic order below $T_{N}^\text{Ir}\sim$ 71 K, consistent with the expected signal of all-in all-out (AIAO) magnetic order. Using a single-ion model to calculate REXS cross-sections, we estimate an ordered magnetic moment of $μ_{5d}^{\text{Ir}} \approx 0.34(3)\,μ_B$ at 5 K. At the Tb $M_5$ edge, long-range ${\bf k}={\bf 0}$ magnetic order appeared below $\sim40$ K, also consistent with an AIAO magnetic structure on the Tb site. Additional insight into the magnetism of the Tb sublattice is gleaned from measurements at the $M_5$ edge in applied magnetic fields up to 6 T, which is found to completely suppress the Tb AIAO magnetic order. In zero applied field, the observed gradual onset of the Tb sublattice magnetisation with temperature suggests that it is induced by the magnetic order on the Ir site. The persistence of AIAO magnetic order, despite the greatly reduced ordering temperature and moment size compared to stoichiometric Tb$_{2}$Ir$_{2}$O$_{7}$, for which $T_{N}^{\text{Ir}} =130$ K and $μ_{5d}^{\text{Ir}}=0.56\,μ_B$, indicates that stuffing could be a viable means of tuning the strength of electronic correlations, thereby potentially offering a new strategy to achieve topologically non-trivial band crossings in pyrochlore iridates.

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arXiv2019

Momentum-resolved lattice dynamics of parent and electron-doped Sr$_{2}$IrO$_{4}$

The mixing of orbital and spin character in the wave functions of the $5d$ iridates has led to predictions of strong couplings among their lattice, electronic and magnetic degrees of freedom. As well as realizing a novel spin-orbit assisted Mott-insulating ground state, the perovskite iridate Sr$_{2}$IrO$_{4}$ has strong similarities with the cuprate La$_{2}$CuO$_{4}$, which on doping hosts a charge-density wave that appears intimately connected to high-temperature superconductivity. These phenomena can be sensitively probed through momentum-resolved measurements of the lattice dynamics, made possible by meV-resolution inelastic x-ray scattering. Here we report the first such measurements for both parent and electron-doped Sr$_{2}$IrO$_{4}$. We find that the low-energy phonon dispersions and intensities in both compounds are well described by the same nonmagnetic density functional theory calculation. In the parent compound, no changes of the phonons on magnetic ordering are discernible within the experimental resolution, and in the doped compound no anomalies are apparent due to charge-density waves. These measurements extend our knowledge of the lattice properties of (Sr$_{1-x}$La$_{x}$)$_{2}$IrO$_{4}$ and constrain the couplings of the phonons to magnetic and charge order.

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arXiv2019

Pressure-induced structural dimerization in the hyperhoneycomb iridate $β$-Li$_2$IrO$_3$ at low temperatures

A pressure-induced collapse of magnetic ordering in $β$-Li$_2$IrO$_3$ at $P_m\sim1.5- 2$ GPa has previously been interpreted as evidence for possible emergence of spin liquid states in this hyperhoneycomb iridate, raising prospects for experimental realizations of the Kitaev model. Based on structural data obtained at \emph{room temperature}, this magnetic transition is believed to originate in small lattice perturbations that preserve crystal symmetry, and related changes in bond-directional anisotropic exchange interactions. Here we report on the evolution of the crystal structure of $β$-Li$_2$IrO$_3$ under pressure at low temperatures ($T\leq50$ K) and show that the suppression of magnetism coincides with a change in lattice symmetry involving Ir-Ir dimerization. The critical pressure for dimerization shifts from 4.4(2) GPa at room temperature to $\sim1.5-2$ GPa below 50 K. While a direct $Fddd \rightarrow C2/c$ transition is observed at room temperature, the low temperature transitions involve new as well as coexisting dimerized phases. Further investigation of the Ir ($L_3$/$L_2$) isotropic branching ratio in x-ray absorption spectra indicates that the previously reported departure of the electronic ground state from a $J_{\rm{eff}}=1/2$ state is closely related to the onset of dimerized phases. In essence, our results suggest that the predominant mechanism driving the collapse of magnetism in $β$-Li$_2$IrO$_3$ is the pressure-induced formation of Ir$_2$ dimers in the hyperhoneycomb network. The results further confirm the instability of the $J_{\rm{eff}}=1/2$ moments and related non-collinear spiral magnetic ordering against formation of dimers in the low-temperature phase of compressed $β$-Li$_2$IrO$_3$.

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arXiv2019

Critical fluctuations in the spin-orbit Mott insulator Sr$_3$Ir$_2$O$_7$

X-ray magnetic critical scattering measurements and specific heat measurements were performed on the perovskite iridate Sr$_3$Ir$_2$O$_7$. We find that the magnetic interactions close to the Néel temperature $T_N$ = 283.4(2) K are three-dimensional. This contrasts with previous studies which suggest two-dimensional behaviour like Sr$_2$IrO$_4$. Violation of the Harris criterion ($dν>2$) means that weak disorder becomes relevant. This leads a rounding of the antiferromagnetic phase transition at $T_N$, and modifies the critical exponents relative to the clean system. Specifically, we determine that the critical behaviour of Sr$_3$Ir$_2$O$_7$ is representative of the diluted 3D Ising universality class.

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arXiv2019

Crossover from itinerant to localized magnetic excitations through the metal-insulator transition in NaOsO$_{\text{3}}$

NaOsO$_{\text{3}}$ undergoes a metal-insulator transition (MIT) at 410 K, concomitant with the onset of antiferromagnetic order. The excitation spectra have been investigated through the MIT by resonant inelastic x-ray scattering (RIXS) at the Os L$_{\text{3}}$ edge. Low resolution ($ΔE \sim$ 300 meV) measurements over a wide range of energies reveal that local electronic excitations do not change appreciably through the MIT. This is consistent with a picture in which structural distortions do not drive the MIT. In contrast, high resolution ($ΔE \sim $ 56 meV) measurements show that the well-defined, low energy magnons in the insulating state weaken and dampen upon approaching the metallic state. Concomitantly, a broad continuum of excitations develops which is well described by the magnetic fluctuations of a nearly antiferromagnetic Fermi liquid. By revealing the continuous evolution of the magnetic quasiparticle spectrum as it changes its character from itinerant to localized, our results provide unprecedented insight into the nature of the MIT in \naoso. In particular, the presence of weak correlations in the paramagnetic phase implies a degree of departure from the ideal Slater limit.

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arXiv2019

Tuning of the Ru$^{\mathbf{4+}}$ ground-state orbital population in the $\mathbf{4d^4}$ Mott insulator Ca$_2$RuO$_4$ achieved by La doping

The ground-state orbital occupancy of the Ru$^{4+}$ ion in Ca$_{2-x}$La$_x$RuO$_4$ [x=0, 0.05(1), 0.07(1) and 0.12(1)] was investigated by performing X-ray absorption spectroscopy (XAS) in the vicinity of the O K edge as a function of angle between the incident beam and the surface of the crystals. A minimal model of the hybridization between the O 2p states probed at the K edge and the Ru 4d orbitals was used to analyze the XAS data, allowing the ratio of hole occupancies $n_{xy}/n_{yz,zx}$ to be determined as a function of doping and temperature. For the samples displaying a low-temperature insulating ground-state ($x\leq0.07$), $n_{xy}/n_{yz,zx}$ is found to increase significantly with increasing doping. For x=0.12, which has a metallic ground-state, the XAS spectra are found to be independent of temperature, and not to be describable by the minimal hybridization model. To understand the origin of the evolution of the electronic structure across the phase diagram, we have performed theoretical calculations based on a model Hamiltonian, comprising electron-electron correlations, crystal field ($Δ$) and spin-orbit coupling ($λ$), of a Ru-O-Ru cluster. Our calculations of the Ru hole occupancy as a function of $Δ/λ$ establish that the enhancement of $n_{xy}/n_{yz,zx}$ is driven by significant changes to the crystal field as the tetragonal distortion of the RuO$_6$ octahedral changes from compressive to tensile with La doping. It also shows that the hole occupancy of the O 2p and Ru 4d orbitals display the same trend as a function of $Δ/λ$, thus validating the minimal hybridization model. In essence, our results suggest that the predominant mechanism driving the emergence of the low-temperature metallic phase in La doped Ca$_2$RuO$_4$ is the structurally induced redistribution of holes within the t2g orbitals, rather that the injection of free carriers.

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arXiv2018

Evidence for $J_{\rm eff} = 0$ ground state and defect-induced spin glass behaviour in the pyrochlore osmate Y$_{2}$Os$_{2}$O$_{7}$

We present AC and DC magnetometry, heat capacity, muon spin relaxation ($μ$SR) and resonant inelastic X-ray scattering (RIXS) studies of the pyrochlore osmate Y$_2$Os$_2$O$_7$. We observe a non-zero effective moment governed by $\sqrt{f}μ_{\rm{eff}} = 0.417(1)\,μ_{\rm{B}}$ where $f$ is the fraction of Os sites which exhibit a spin, and spin freezing at temperature $T_{\rm f} \simeq 5\,$K, consistent with previous results. The field dependence of magnetisation data shows that the paramagnetic moment is most likely due to large moments $μ_{\rm eff} \simeq 3\,μ_{\rm B}$ on only a small fraction $f \simeq 0.02$ of Os sites. Comparison of single-ion energy level calculations with the RIXS data yields a non-magnetic $J_{\rm eff} = 0$ ground state on the Os$^{4+}$ sites. The spin-orbit interaction, Hund's coupling and trigonal distortion of OsO$_{6}$ octahedra are all important in modelling the experimentally observed spectra. We are able to rule out impurity effects, leaving disorder-related effects such as oxygen non-stoichiometry or site interchange between Os and Y ions as the most plausible explanation for the magnetic response in this material.

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