arXiv subjects

J. P. Clancy

Publications and source records attributed to J. P. Clancy.

At least 37 records · Page 2Linked to original sources

arXiv2018

Probing electronic excitations in iridates with resonant inelastic x-ray scattering and emission spectroscopy techniques

We report a comprehensive resonant inelastic x-ray scattering (RIXS) study of various iridate materials focusing on core-level excitations and transitions between crystal-field split d-levels. The 2p core hole created at the Ir $L_3$ absorption edge has a very short lifetime giving rise to a broad absorption width ($\sim 5$~eV). This absorption linewidth broadening can be overcome by studying the resonant x-ray emission spectroscopy (RXES) map, which is a two-dimensional intensity map of the Ir L$α_2$ emission obtained with high energy-resolution monochromator and analyzer. By limiting the emitted photon energy to a narrow range, one can obtain x-ray absorption spectra in the high energy-resolution fluorescence detection (HERFD) mode, while one can also simulate quasi-$M_4$-edge absorption spectra by integrating over incident photon energies. Both methods improve the absorption line width significantly, allowing detailed studies of unoccupied electronic structure in iridates and other $5d$ transition metal compounds. On the other hand, the short lifetime of the 2p core hole benefits the study of excitations of valence electrons. We show that the incident energy dependence of the RIXS spectra for $d-d$ transitions is simple to understand due to the short core-hole lifetime, which validates ultra-short core-hole lifetime approximation used widely in theoretical calculations. We compared $d-d$ excitations in various iridates and found that the excitations between the t$_{2g}$ and e$_g$ states share many similarities among different materials. However, the RIXS spectra due to the transitions between the spin-orbit-split t$_{2g}$ levels vary widely depending on the oxidation state and electronic bandwidths.

cond-mat.str-el↗

arXiv2018

Pressure-driven collapse of the relativistic electronic ground state in a honeycomb iridate

The electronic ground state in many iridate materials is described by a complex wave-function in which spin and orbital angular momenta are entangled due to relativistic spin-orbit coupling (SOC). Such a localized electronic state carries an effective total angular momentum of $J_{eff}=1/2$. In materials with an edge-sharing octahedral crystal structure, such as the honeycomb iridates Li2IrO3 and Na2IrO3, these $J_{eff}=1/2$ moments are expected to be coupled through a special bond-dependent magnetic interaction, which is a necessary condition for the realization of a Kitaev quantum spin liquid. However, this relativistic electron picture is challenged by an alternate description, in which itinerant electrons are confined to a benzene-like hexagon, keeping the system insulating despite the delocalized nature of the electrons. In this quasi-molecular orbital (QMO) picture, the honeycomb iridates are an unlikely choice for a Kitaev spin liquid. Here we show that the honeycomb iridate Li2IrO3 is best described by a $J_{eff}=1/2$ state at ambient pressure, but crosses over into a QMO state under the application of small (~ 0.1 GPa) hydrostatic pressure. This result illustrates that the physics of iridates is extremely rich due to a delicate balance between electronic bandwidth, spin-orbit coupling, crystal field, and electron correlation.

cond-mat.str-el↗

arXiv2017

Determination of Hund's coupling in 5d Oxides using Resonant Inelastic X-ray Scattering

We report resonant inelastic X-ray scattering (RIXS) measurements on ordered double perovskite samples containing Re$^{5+}$ and Ir$^{5+}$ with $5d^2$ and $5d^4$ electronic configurations respectively. In particular, the observed RIXS spectra of Ba$_2$YReO$_6$ and Sr$_2$MIrO$_6$ (M=Y, Gd) show sharp intra-t$_{2g}$ transitions, which can be quantitatively understood using a minimal `atomic' Hamiltonian incorporating spin-orbit coupling ($λ$) and Hund's coupling ($J_H$). Our analysis yields $λ=0.38(2)$eV with $J_H=0.26(2)$eV for Re$^{5+}$, and $λ=0.42(2)$eV with $J_H=0.25(4)$eV for Ir$^{5+}$. Our results provide the first sharp estimates for the Hund's coupling in $5d$ oxides, and suggest that it should be treated on equal footing with spin-orbit interaction in multi-orbital $5d$ transition metal compounds.

cond-mat.str-el↗

arXiv2016

Disordered dimer state in electron-doped Sr$_{3}$Ir$_{2}$O$_{7}$

Spin excitations are explored in the electron-doped spin-orbit Mott insulator (Sr$_{1-x}$La$_{x}$)$_3$Ir$_2$O$_7$. As this bilayer square lattice system is doped into the metallic regime, long-range antiferromagnetism vanishes, yet a spectrum of gapped spin excitation remains. Excitation lifetimes are strongly damped with increasing carrier concentration, and the energy integrated spectral weight becomes nearly momentum independent as static spin order is suppressed. Local magnetic moments, absent in the parent system, grow in metallic samples and approach values consistent with one $J=\frac{1}{2}$ impurity per electron doped. Our combined data suggest that the magnetic spectra of metallic (Sr$_{1-x}$La$_{x}$)$_3$Ir$_2$O$_7$ are best described by excitations out of a disordered dimer state.

cond-mat.str-el↗

arXiv2015

X-ray scattering study of pyrochlore iridates: crystal structure, electronic and magnetic excitations

We have investigated the structural, electronic, and magnetic properties of the pyrochlore iridates Eu2Ir2O7 and Pr2Ir2O7 using a combination of resonant elastic x-ray scattering, x-ray powder diffraction, and resonant inelastic x-ray scattering (RIXS). The structural parameters of Eu2Ir2O7 have been examined as a function of temperature and applied pressure, with a particular emphasis on regions of the phase diagram where electronic and magnetic phase transitions have been reported. We find no evidence of crystal symmetry change over the range of temperatures (~6 to 300 K) and pressures (~0.1 to 17 GPa) studied. We have also investigated the electronic and magnetic excitations in single crystal samples of Eu2Ir2O7 and Pr2Ir2O7 using high resolution Ir L3-edge RIXS. In spite of very different ground state properties, we find these materials exhibit qualitatively similar excitation spectra, with crystal field excitations at ~3-5 eV, spin-orbit excitations at ~0.5-1 eV, and broad low-lying excitations below ~0.15 eV. In Eu2Ir2O7 we observe highly damped magnetic excitations at ~45 meV, which display significant momentum dependence. We compare these results with recent dynamical structure factor calculations.

cond-mat.str-el↗

arXiv2015

Topological states in pyrochlore iridates: long-range anisotropy strongly competing with spin-orbit interaction

In the search for topological phases in correlated electron systems, iridium-based pyrochlores A2Ir2O7 -- materials with 5d transition-metal ions -- provide fertile grounds. Several novel topological states have been predicted but the actual realization of such states is believed to critically depend on the strength of local potentials arising from distortions of IrO6-cages. We test this hypothesis by measuring with resonant x-ray scattering the electronic level splittings in the A= Y, Eu systems, which we show to agree very well with ab initio electronic structure calculations. We find, however, that not distortions of IrO6-octahedra are the primary source for quenching the spin-orbit interaction, but strong long-range lattice anisotropies, which inevitably break the local cubic symmetry and will thereby be decisive in determining the system's topological ground state.

cond-mat.str-el↗

arXiv2015

Magnetic order in $α$-RuCl$_3$: a honeycomb lattice quantum magnet with strong spin-orbit coupling

We report magnetic and thermodynamic properties of single crystal $α$-RuCl$_3$, in which the Ru$^{3+}$ ($4d^5$) ion is in its low spin state and forms a honeycomb lattice. Two features are observed in both magnetic susceptibility and specific heat data; a sharp peak at 7~K and a broad hump near 10-15K. In addition, we observe a metamagnetic transition between 5~T and 10~T. Our neutron diffraction study of single crystal samples confirms that the low temperature peak in the specific heat is associated with a magnetic order with unit cell doubling along the honeycomb (100) direction, which is consistent with zigzag order, one of the types of magnetic order predicted within the framework of the Kitaev-Heisenberg model.

cond-mat.str-el↗

arXiv2014

Tuning Magnetic Coupling in Sr$_2$IrO$_4$ Thin Films with Epitaxial Strain

We report x-ray resonant magnetic scattering (XRMS) and resonant inelastic x-ray scattering (RIXS) studies of epitaxially-strained $\mathrm{Sr_2IrO_4}$ thin films. The films were grown on $\mathrm{SrTiO_3}$ and $\mathrm{(LaAlO_3)_{0.3}(Sr_2AlTaO_6)_{0.7}}$ substrates, under slight tensile and compressive strains, respectively. Although the films develop a magnetic structure reminiscent of bulk $\mathrm{Sr_2IrO_4}$, the magnetic correlations are extremely anisotropic, with in-plane correlation lengths significantly longer than the out-of-plane correlation lengths. In addition, the compressive (tensile) strain serves to suppress (enhance) the magnetic ordering temperature $\mathrm{T_N}$, while raising (lowering) the energy of the zone boundary magnon. Quantum chemical calculations show that the tuning of magnetic energy scales can be understood in terms of strain-induced change in bond lengths.

cond-mat.str-el↗

arXiv2014

Sudden reversal in the pressure dependence of Tc in the iron-based superconductor CsFe2As2: A possible link between inelastic scattering and pairing symmetry

We report a sudden reversal in the pressure dependence of Tc in the iron-based superconductor CsFe2As2, similar to that discovered recently in KFe2As2 [Tafti et al., Nat. Phys. 9, 349 (2013)]. As in KFe2As2, we observe no change in the Hall coefficient at the zero temperature limit, again ruling out a Lifshitz transition across the critical pressure Pc. We interpret the Tc reversal in the two materials as a phase transition from one pairing state to another, tuned by pressure, and investigate what parameters control this transition. Comparing samples of different residual resistivity, we find that a 6-fold increase in impurity scattering does not shift Pc. From a study of X-ray diffraction on KFe2As2 under pressure, we report the pressure dependence of lattice constants and As-Fe-As bond angle. The pressure dependence of these lattice parameters suggests that Pc should be significantly higher in CsFe2As2 than in KFe2As2, but we find on the contrary that Pc is lower in CsFe2As2. Resistivity measurements under pressure reveal a change of regime across Pc, suggesting a possible link between inelastic scattering and pairing symmetry.

cond-mat.supr-con↗

arXiv2014

$α$-RuCl3: a Spin-Orbit Assisted Mott Insulator on a Honeycomb Lattice

We examine the role of spin-orbit coupling in the electronic structure of $α$-RuCl3, in which Ru ions in 4d5 configuration form a honeycomb lattice. The measured optical spectra exhibit a clear optical gap and excitations within the t2g orbitals. The spectra can be described very well with first-principles electronic structure calculations obtained by taking into account both spin orbit coupling and electron correlations. Furthermore, our X-ray absorption spectroscopy measurements at the Ru L-edges exhibit distinct spectral features associated with the presence of substantial spin- orbit coupling, as well as an anomalously large branching ratio. We propose that $α$-RuCl3 is a spin-orbit assisted Mott insulator, and the bond-dependent Kitaev interaction may be relevant for this compound.

cond-mat.str-el↗

arXiv2014

Dilute Magnetism and Spin-Orbital Percolation Effects in Rh-doped Sr2IrO4

We have used a combination of resonant magnetic x-ray scattering (RMXS) and x-ray absorption spectroscopy (XAS) to investigate the properties of the doped spin-orbital Mott insulator Sr2Ir(1-x)Rh(x)O4 (0.07 < x < 0.70). We show that Sr2Ir(1-x)Rh(x)O4 represents a unique model system for the study of dilute magnetism in the presence of strong spin-orbit coupling, and provide evidence of a doping-induced change in magnetic structure and a suppression of magnetic order at x_c ~ 0.17. We demonstrate that Rh-doping introduces Rh3+/Ir5+ ions which effectively hole-dope this material. We propose that the magnetic phase diagram for this material can be understood in terms of a novel spin-orbital percolation picture.

cond-mat.str-el↗

arXiv2013

Spin Gap and the Nature of the 4d3 Magnetic Ground State in the Frustrated FCC Antiferromagnet Ba2YRuO6

The geometrically frustrated double perovskite Ba2YRuO6 has magnetic 4d3 Ru5+ ions decorating an undistorted face-centered cubic (FCC) lattice. This material has been previously reported to exhibit commensurate long-range antiferromagnetic order below T_N = 36K, a factor f = 15 times lower than its Curie-Weiss temperature Theta_CW = -522 K, and purported short-range order to T* = 47K. We report new time-of-flight neutron spectroscopy of Ba2YRuO6 which shows the development of a 5 meV spin gap in the vicinity of the [100] magnetic ordering wavevector below T_N = 36K, with the transition to long-range order occurring at T* = 47K. We also report spin waves extending to 14 meV, a surprisingly small bandwidth in light of the large Theta_CW. We compare the spin gap and bandwidth to relevant neutron studies of the isostructural 4d1 material Ba2YMoO6,and discuss the results in the framework of relatively strong spin-orbit coupling expected in 4d magnetic systems.

cond-mat.str-el↗

arXiv2013

Magnetic excitation spectrum of Na2IrO3 probed with resonant inelastic x-ray scattering

The low energy excitations in Na2IrO3 have been investigated using resonant inelastic x-ray scattering (RIXS). A magnetic excitation branch can be resolved, whose dispersion reaches a maximum energy of about 35 meV at the Γ-point. The momentum dependence of the excitation energy is much larger along the Γ-X direction compared to that along the Γ-Y direction. The observed dispersion relation is consistent with a recent theoretical prediction based on Heisenberg-Kitaev model. At high temperatures, we find large contributions from lattice vibrational modes to our RIXS spectra, suggesting that a strong electron-lattice coupling is present in Na2IrO3.

cond-mat.str-el↗

arXiv2013

Spin-orbital locked magnetic excitations in a half-metallic double perovskite Ba2FeReO6

We present a powder inelastic neutron scattering study of magnetic excitations in Ba$_2$FeReO$_6$, a member of the double perovskite family of materials which exhibit half-metallic behavior and high Curie temperatures. We find clear evidence of two well-defined dispersing magnetic modes in its low temperature ferrimagnetic state. We develop a local moment model, which incorporates the interaction of Fe spins with spin-orbit locked magnetic moments on Re, and show that this captures our experimental observations. Our study further opens up double perovskites as model systems to explore the interplay of strong correlations and spin-orbit coupling in 5d transition metal oxides.

cond-mat.str-el↗

arXiv2012

Crystal field splitting and correlation effect on the electronic structure of A2IrO3

The electronic structure of the honeycomb lattice iridates Na2IrO3 and Li2IrO3 has been investigated using resonant inelastic x-ray scattering (RIXS). Crystal-field split d-d excitations are resolved in the high-resolution RIXS spectra. In particular, the splitting due to non-cubic crystal fields, derived from the splitting of j_eff=3/2 states, is much smaller than the typical spin-orbit energy scale in iridates, validating the applicability of j_eff physics in A2IrO3. We also find excitonic enhancement of the particle-hole excitation gap around 0.4 eV, indicating that the nearest-neighbor Coulomb interaction could be large. These findings suggest that both Na2IrO3 and Li2IrO3 can be described as spin-orbit Mott insulators, similar to the square lattice iridate Sr2IrO4.

cond-mat.str-el↗

arXiv2012

Field-induced magnetic behavior of the bilayer iridate Sr3Ir2O7

We have performed resonant magnetic x-ray scattering (RMXS) measurements on single crystal samples of the bilayer iridate Sr3Ir2O7. We observe the development of antiferromagnetic order below T* ~ 260 K, which persists down to T = 4 K under both field-cooled (fc) and zero-field-cooled (zfc) conditions. The temperature dependence of the fc and zfc magnetic Bragg peaks suggests the presence of competition between canted and collinear antiferromagnetic ground states. Under zfc conditions, we observe a suppression of magnetic peak intensity at T_D ~ 50 K which can be attributed to a spin reorientation transition. Under fc conditions, we find that the canted antiferromagnetic state is stabilized over a much wider range of temperatures, with significantly enhanced magnetic correlation lengths within the Ir-O layers. The field dependence of the magnetic Bragg peaks provides no evidence of field-induced phase transitions for H < 4 T.

cond-mat.str-el↗

arXiv2012

Spin-Orbit Coupling in Iridium-Based 5d Compounds Probed by X-ray Absorption Spectroscopy

We have performed x-ray absorption spectroscopy (XAS) measurements on a series of Ir-based 5d transition metal compounds, including Ir, IrCl3, IrO2, Na2IrO3, Sr2IrO4, and Y2Ir2O7. By comparing the intensity of the "white-line" features observed at the Ir L2 and L3 absorption edges, it is possible to extract valuable information about the strength of the spin-orbit coupling in these systems. We observe remarkably large, non-statistical branching ratios in all Ir compounds studied, with little or no dependence on chemical composition, crystal structure, or electronic state. This result confirms the presence of strong spin-orbit coupling effects in novel iridates such as Sr2IrO4, Na2IrO3, and Y2Ir2O7, and suggests that even simple Ir-based compounds such as IrO2 and IrCl3 may warrant further study. In contrast, XAS measurements on Re-based 5d compounds, such as Re, ReO2, ReO3, and Ba2FeReO6, reveal statistical branching ratios and negligible spin-orbit coupling effects.

cond-mat.str-el↗

arXiv2012

High resolution x-ray scattering studies of structural phase transitions in Cr-doped BaFe2As2

We have performed high resolution x-ray scattering measurements on single crystal samples of Ba(Fe(1-x)Cr(x))2As2 (x = 0 to 0.335). These measurements examine the effect of Cr-doping on the high temperature tetragonal (I4/mmm) to low temperature orthorhombic (Fmmm) structural phase transition of the parent compound BaFe2As2. Increasing Cr concentration is found to suppress the structural transition temperature (Ts), and reduce the magnitude of the orthorhombic strain (delta). The doping dependence of the orthorhombic strain, combined with complementary measurements of the high temperature magnetic susceptibility, suggests the presence of a magnetostructural crossover at x ~ 0.05. In particular, this crossover appears to mark a shift from strong to weak orthorhombicity and from predominantly itinerant to localized magnetic behavior.

cond-mat.str-el↗