arXiv subjects

M. H. Upton

Publications and source records attributed to M. H. Upton.

At least 19 recordsLinked to original sources

arXiv2023

Local site behavior of the 5d and 4f ions in the frustrated pyrochlore Ho2Os2O7

The pyrochlore osmate Ho2Os2O7 is a candidate material for a fragile J=0 local singlet ground state, however little is known regarding the single-ion behavior of either the Os or Ho ions. To address this we present polarized neutron powder diffraction (PNPD) and resonant inelastic x-ray scattering (RIXS) measurements that separately probe the local site behavior of the Os and Ho ions. The PNPD results are dominated by Ho3+ scattering and the analysis reveals local site susceptibility behavior consistent with spin ice materials. Complimentary unpolarized neutron powder diffraction show an ordered spin ice ground state in an applied magnetic field. To isolate the Os4+ single-ion behavior we present resonant inelastic x-ray scattering (RIXS) measurements at the osmium L-edge. Analysis of the RIXS spectra parameterize the spin-orbit coupling (0.35 eV), Hund's coupling (0.27 eV) and trigonal distortion (-0.17 eV). The results are considered within the context of a J=0 model and possible departures from this through structural distortions, excitonic interactions and 5d-4f interactions between the Os ion and the surrounding Ho lattice. The experimental methodology employed highlights the complimentary information available in rare earth based 5d pyrochlores from distinct neutron and x-ray scattering techniques that allow for the isolation and determination of the behavior of the different ions.

cond-mat.str-el↗

arXiv2023

Quasimolecular $J_{\rm tet}$=3/2 moments in the cluster Mott insulator GaTa$_4$Se$_8$

Quasimolecular orbitals in cluster Mott insulators provide a route to tailor exchange interactions, which may yield novel quantum phases of matter. We demonstrate the cluster Mott character of the lacunar spinel GaTa$_4$Se$_8$ using resonant inelastic x-ray scattering (RIXS) at the Ta $L_3$ edge. Electrons are fully delocalized over Ta$_4$ tetrahedra, forming quasimolecular $J_{\rm tet}$=3/2 moments. The modulation of the RIXS intensity as function of the transferred momentum q allows us to determine the cluster wavefunction, which depends on competing intracluster hopping terms that mix states with different character. This mixed wavefunction is decisive for the macroscopic properties since it affects intercluster hopping and exchange interactions and furthermore renormalizes the effective spin-orbit coupling constant. The versatile wavefunction, tunable via intracluster hopping, opens a new perspective on the large family of lacunar spinels and cluster Mott insulators in general.

cond-mat.str-el↗

arXiv2023

Evolution of plasmon excitations across the phase diagram of the cuprate superconductor La$_{2-x}$Sr$_{x}$CuO$_4$

We use resonant inelastic x-ray scattering (RIXS) at the O $K$- and Cu $K$-edges to investigate the doping- and temperature dependence of low-energy plasmon excitations in La$_{2-x}$Sr$_{x}$CuO$_4$. We observe a monotonic increase of the energy scale of the plasmons with increasing doping $x$ in the underdoped regime, whereas a saturation occurs above optimal doping $x \gtrsim 0.16$ and persists at least up to $x = 0.4$. Furthermore, we find that the plasmon excitations show only a marginal temperature dependence, and possible effects due to the superconducting transition and the onset of strange metal behavior are either absent or below the detection limit of our experiment. Taking into account the strongly correlated character of the cuprates, we show that layered $t$-$J$-$V$ model calculations accurately capture the increase of the plasmon energy in the underdoped regime. However, the computed plasmon energy continues to increase even for doping levels above $x \gtrsim 0.16$, which is distinct from the experimentally observed saturation, and reaches a broad maximum around $x = 0.55$. We discuss whether possible lattice disorder in overdoped samples, a renormalization of the electronic correlation strength at high dopings, or an increasing relevance of non-planar Cu and O orbitals could be responsible for the discrepancy between experiment and theory for doping levels above $x = 0.16$.

cond-mat.supr-con↗

arXiv2023

Momentum-independent magnetic excitation continuum in the honeycomb iridate H$_3$LiIr$_2$O$_6$

In the search for realizations of Quantum Spin Liquids (QSL), it is essential to understand the interplay between inherent disorder and the correlated fluctuating spin ground state. H$_3$LiIr$_2$O$_6$ is regarded as a spin liquid proximate to the Kitaev-limit (KQSL) in which H zero-point motion and stacking faults are known to be present. Bond disorder has been invoked to account for the existence of unexpected low-energy spin excitations. Controversy remains about the nature of the underlying correlated state and if any KQSL physics survives. Here, we use resonant X-ray spectroscopies to map the collective excitations in H$_3$LiIr$_2$O$_6$ and characterize its magnetic state. We uncover a broad bandwidth and momentum-independent continuum of magnetic excitations at low temperatures that are distinct from the paramagnetic state. The center energy and high-energy tail of the continuum are consistent with expectations for dominant ferromagnetic Kitaev interactions between dynamically fluctuating spins. The absence of a momentum dependence to these excitations indicates a broken translational invariance. Our data support an interpretation of H$_3$LiIr$_2$O$_6$ as a disordered topological spin liquid in close proximity to bond-disordered versions of the KQSL. Our results shed light on how random disorder affects topological magnetic states and have implications for future experimental and theoretical works toward realizing the Kitaev model in condensed matter systems

cond-mat.str-el↗

arXiv2023

RIXS observation of bond-directional nearest-neighbor excitations in the Kitaev material Na$_2$IrO$_3$

Spin-orbit coupling locks spin direction and spatial orientation and generates, in semi-classical magnets, a local spin easy-axis and associated ordering. Quantum spin-1/2's defy this fate: rather than spins becoming locally anisotropic, the spin-spin interactions do. Consequently interactions become dependent on the spatial orientation of bonds between spins, prime theoretical examples of which are Kitaev magnets. Bond-directional interactions imply the existence of bond-directional magnetic modes, predicted spin excitations that render crystallographically equivalent bonds magnetically inequivalent, which yet have remained elusive experimentally. Here we show that resonant inelastic x-ray scattering allows us to explicitly probe the bond-directional character of magnetic excitations. To do so, we use a scattering plane spanned by one bond and the corresponding spin component and scan a range of momentum transfer that encompasses multiple Brillouin zones. Applying this approach to Na$_2$IrO$_3$ we establish the different bond-directional characters of magnetic excitations at 10 meV and 45 meV. Combined with the observation of spin-spin correlations that are confined to a single bond, this experimentally validates the Kitaev character of exchange interactions long proposed for this material.

cond-mat.str-el↗

arXiv2022

Spin-orbit coupling controlled ground states in the double perovskite iridates A2BIrO6 (A = Ba, Sr; B = Lu, Sc)

Iridates with the 5$d^4$ electronic configuration have attracted recent interest due to reports of magnetically-ordered ground states despite longstanding expectations that their strong spin-orbit coupling would generate a $J = 0$ electronic ground state for each Ir$^{5+}$ ion. The major focus of prior research has been on the double perovskite iridates Ba$_2$YIrO$_6$ and Sr$_2$YIrO$_6$, where the nature of the ground states (i.e. ordered vs non-magnetic) is still controversial. Here we present neutron powder diffraction, high energy resolution fluorescence detected x-ray absorption spectroscopy (HERFD-XAS), resonant inelastic x-ray scattering (RIXS), magnetic susceptibility, and muon spin relaxation data on the related double perovskite iridates Ba$_2$LuIrO$_6$, Sr$_2$LuIrO$_6$, Ba$_2$ScIrO$_6$, and Sr$_2$ScIrO$_6$ that enable us to gain a general understanding of the electronic and magnetic properties for this family of materials. Our HERFD-XAS and RIXS measurements establish $J = 0$ electronic ground states for the Ir$^{5+}$ ions in all cases, with similar values for Hund's coupling $J_{\rm H}$ and the spin-orbit coupling constant $λ_{\rm SOC}$. Our bulk susceptibility and muon spin relaxation data find no evidence for long-range magnetic order or spin freezing, but they do reveal weak magnetic signals that are consistent with extrinsic local moments. Our results indicate that the large $λ_{\rm SOC}$ is the key driving force behind the electronic and magnetic ground states realized in the 5$d^4$ double perovskite iridates, which agrees well with conventional wisdom.

cond-mat.str-el↗

arXiv2022

On the electronic ground state of two non-magnetic pentavalent honeycomb iridates

We investigate the electronic structure of two Ir$^{5+}$ honeycomb iridates, Sr$_3$CaIr$_2$O$_9$ and NaIrO$_3$, by means of resonant x-ray techniques. We confirm that Sr$_3$CaIr$_2$O$_9$ realizes a large spin-orbit driven non-magnetic $J = 0$ singlet ground state despite sizable tetragonal distortions of Ir coordinating octahedra. On the other hand, the resonant inelastic x-ray spectra of NaIrO$_3$ are drastically different from expectations for a Mott insulator with octahedrally coordinated Ir$^{5+}$. We find that the data for NaIrO$_3$ can be best interpreted as originating from a narrow gap non-magnetic $S = 0$ band insulating ground state. Our results highlight the complex role of the ligand environment in the electronic structure of honeycomb iridates and the essential role of x-ray spectroscopy to characterize electronic ground states of insulating materials.

cond-mat.str-el↗

arXiv2022

Magnetic Excitations in Square Lattice Iridates: Contrast between Ba$_2$IrO$_4$ and Sr$_2$IrO$_4$

We report a resonant inelastic x-ray scattering (RIXS) investigation of ultra-thin epitaxial films of Ba$_2$IrO$_4$, and compare their low energy magnetic and spin-orbit excitations to those of their sister compound Sr$_2$IrO$_4$. Due to the 180$^\circ$ Ir-O-Ir bond, the bandwidth of the magnon and spin-orbiton is significantly larger in Ba$_2$IrO$_4$, making it difficult to describe these two types of excitations as separate well-defined quasiparticles. Both types of excitations are found to be quite sensitive to the effect of epitaxial strain. In addition, we find that the d-level inversion observed in Sr$_2$IrO$_4$ is absent in Ba$_2$IrO$_4$, as predicted in recent theoretical studies. Our results illustrate that the magnetic properties of Ba$_2$IrO$_4$ are substantially different from those of Sr$_2$IrO$_4$, suggesting that these materials need to be examined more carefully with electron itinerancy taken into account.

cond-mat.str-el↗

arXiv2022

Antiferromagnetic Excitonic Insulator State in Sr3Ir2O7

Excitonic insulators are usually considered to form via the condensation of a soft charge mode of bound electron-hole pairs. This, however, presumes that the soft exciton is of spin-singlet character. Early theoretical considerations have also predicted a very distinct scenario, in which the condensation of magnetic excitons results in an antiferromagnetic excitonic insulator state. Here we report resonant inelastic x-ray scattering (RIXS) measurements of Sr3Ir2O7. By isolating the longitudinal component of the spectra, we identify a magnetic mode that is well-defined at the magnetic and structural Brillouin zone centers, but which merges with the electronic continuum in between these high-symmetry points and which decays upon heating concurrent with a decrease in the material's resistivity. We show that a bilayer Hubbard model, in which electron-hole pairs are bound by exchange interactions, consistently explains all the electronic and magnetic properties of Sr3Ir2O7 indicating that this material is a realization of the long-predicted antiferromagnetic excitonic insulators phase.

cond-mat.str-el↗

arXiv2021

Nearly itinerant electronic groundstate in the intercalated honeycomb iridate Ag$_3$LiIr$_2$O$_6$

We use x-ray spectroscopy at Ir L$_3$/L$_2$ absorption edge to study powder samples of the intercalated honeycomb magnet Ag$_3$LiIr$_2$O$_6$. Based on x-ray absorption and resonant inelastic x-ray scattering measurements, and exact diagonalization calculations including next-neighbour Ir-Ir electron hoping integrals, we argue that the intercalation of Ag atoms results in a nearly itinerant electronic structure with enhanced Ir-O hybridization. As a result of the departure from the local relativistic $j_{\rm eff}\! = \!1/2$ state, we find that the relative orbital contribution to the magnetic moment is increased, and the magnetization density is spatially extended and asymmetric. Our results confirm the importance of metal - ligand hybridazation in the magnetism of transition metal oxides and provide empirical guidance for understanding the collective magnetism in intercalated honeycomb iridates.

cond-mat.str-el↗

arXiv2021

Relationship between A-site Cation and Magnetic Structure in 3d-5d-4f Double Perovskite Iridates Ln2NiIrO6 (Ln=La, Pr, Nd)

We report a comprehensive investigation of Ln2NiIrO6 (Ln = La, Pr, Nd) using thermodynamic and transport properties, neutron powder diffraction, resonant inelastic x-ray scattering, and density functional theory (DFT) calculations to investigate the role of A-site cations on the magnetic interactions in this family of hybrid 3d-5d-4f compositions. Magnetic structure determination using neutron diffraction reveals antiferromagnetism for La2NiIrO6, a collinear ferrimagnetic Ni/Ir state that is driven to long range antiferromagnetism upon the onset of Nd ordering in Nd2NiIrO6, and a non-collinear ferrimagnetic Ni/Ir sublattice interpenetrated by a ferromagnetic Pr lattice for Pr2NiIrO6. For Pr2NiIrO6 heat capacity results reveal the presence of two independent magnetic sublattices and transport resistivity indicates insulating behavior and a conduction pathway that is thermally mediated. First principles DFT calculation elucidates the existence of the two independent magnetic sublattices within Pr2NiIrO6 and offers insight into the behavior in La2NiIrO6 and Nd2NiIrO6. Resonant inelastic x-ray scattering is consistent with spin-orbit coupling splitting the t2g manifold of octahedral Ir4+ into a Jeff = 1/2 and Jeff = 3/2 state for all members of the series considered.

cond-mat.str-el↗

arXiv2021

Charge ordering in Ir dimers in the ground state of Ba$_5$AlIr$_2$O$_{11}$

It has been well established experimentally that the interplay of electronic correlations and spin-orbit interactions in Ir$^{4+}$ and Ir$^{5+}$ oxides results in insulating J$_{\rm eff}$=1/2 and J$_{\rm eff}$=0 ground states, respectively. However, in compounds where the structural dimerization of iridum ions is favourable, the direct Ir $d$--$d$ hybridisation can be significant and takes a key role. Here, we investigate the effects of direct Ir $d$--$d$ hybridisation in comparison with electronic correlations and spin-orbit coupling in Ba$_5$AlIr$_2$O$_{11}$, a compound with Ir dimers. Using a combination of $ab$ $initio$ many-body wave function quantum chemistry calculations and resonant inelastic X-ray scattering (RIXS) experiments, we elucidate the electronic structure of Ba$_5$AlIr$_2$O$_{11}$. We find excellent agreement between the calculated and the measured spin-orbit excitations. Contrary to the expectations, the analysis of the many-body wave function shows that the two Ir (Ir$^{4+}$ and Ir$^{5+}$) ions in the Ir$_2$O$_9$ dimer unit in this compound preserve their local J$_{\rm eff}$ character close to 1/2 and 0, respectively. The local point group symmetry at each of the Ir sites assumes an important role, significantly limiting the direct $d$--$d$ hybridisation. Our results emphasize that minute details in the local crystal field (CF) environment can lead to dramatic differences in electronic states in iridates and 5$d$ oxides in general.

cond-mat.str-el↗

arXiv2020

Structural, electronic, and magnetic properties of nearly-ideal $J_{\rm eff}$ $=$ 1/2 iridium halides

Heavy transition metal magnets with $J_{\rm eff}$ $=$ 1/2 electronic ground states have attracted recent interest due to their penchant for hosting new classes of quantum spin liquids and superconductors. Unfortunately, model systems with ideal $J_{\rm eff}$ $=$ 1/2 states are scarce due to the importance of non-cubic local distortions in most candidate materials. In this work, we identify a family of iridium halide systems [i.e. K$_2$IrCl$_6$, K$_2$IrBr$_6$, (NH$_4$)$_2$IrCl$_6$, and Na$_2$IrCl$_6 \cdotp $ 6(H$_2$O)] with Ir$^{4+}$ electronic ground states in extremely close proximity to the ideal $J_{\rm eff}$ $=$ 1/2 limit, despite a variation in the low-temperature global crystal structures. We also find ordered magnetic ground states for the three anhydrous systems, with single crystal neutron diffraction on K$_2$IrBr$_6$ revealing Type-I antiferromagnetism. This spin configuration is consistent with expectations for significant Kitaev exchange in a face-centered-cubic magnet.

cond-mat.str-el↗

arXiv2019

Magnetic excitations in hole-doped Sr2IrO4: A comparison with electron-doped cuprates

We have studied the evolution of magnetic and orbital excitations as a function of hole-doping in single crystal samples of Sr2Ir(1-x)Rh(x)O4 (0.07 < x < 0.42) using high resolution Ir L3-edge resonant inelastic x-ray scattering (RIXS). Within the antiferromagnetically ordered region of the phase diagram (x < 0.17) we observe highly dispersive magnon and spin-orbit exciton modes. Interestingly, both the magnon gap energy and the magnon bandwidth appear to increase as a function of doping, resulting in a hardening of the magnon mode with increasing hole doping. As a result, the observed spin dynamics of hole-doped iridates more closely resemble those of the electron-doped, rather than hole-doped, cuprates. Within the paramagnetic region of the phase diagram (0.17 < x < 0.42) the low-lying magnon mode disappears, and we find no evidence of spin fluctuations in this regime. In addition, we observe that the orbital excitations become essentially dispersionless in the paramagnetic phase, indicating that magnetic order plays a crucial role in the propagation of the spin-orbit exciton.

cond-mat.str-el↗

arXiv2019

Revisiting the Kitaev material candidacy of Ir4+ double perovskite iridates

Quantum magnets with significant bond-directional Ising interactions, so-called Kitaev materials, have attracted tremendous attention recently in the search for exotic spin liquid states. Here we present a comprehensive set of measurements that enables us to investigate the crystal structures, Ir$^{4+}$ single ion properties, and magnetic ground states of the double perovskite iridates La$_2B$IrO$_6$ ($B$ $=$ Mg, Zn) and $A_2$CeIrO$_6$ ($A$ $=$ Ba, Sr) with a large nearest neighbor distance $>$ 5 Angstroms between Ir$^{4+}$ ions. Our neutron powder diffraction data on Ba$_2$CeIrO$_6$ can be refined in the cubic space group Fm$\bar{3}$m, while the other three systems are characterized by weak monoclinic structural distortions. Despite the variance in the non-cubic crystal field experienced by the Ir$^{4+}$ ions in these materials, X-ray absorption spectroscopy and resonant inelastic x-ray scattering are consistent with $J_{\rm eff}$ $=$ 1/2 moments in all cases. Furthermore, neutron scattering and resonant magnetic x-ray scattering show that these systems host A-type antiferromagnetic order. These electronic and magnetic ground states are consistent with expectations for face-centered-cubic magnets with significant antiferromagnetic Kitaev exchange, which indicates that spacing magnetic ions far apart may be a promising design principle for uncovering additional Kitaev materials.

cond-mat.str-el↗

arXiv2018

Direct detection of dimer orbitals in Ba$_5$AlIr$_2$O$_{11}$

The electronic states of many Mott insulators, including iridates, are often conceptualized in terms of localized atomic states such as the famous "$J_\text{eff}=1/2$ state". Although, orbital hybridization can strongly modify such states and dramatically change the electronic properties of materials, probing this process is highly challenging. In this work, we directly detect and quantify the formation of dimer orbitals in an iridate material Ba$_5$AlIr$_2$O$_{11}$ using resonant inelastic x-ray scattering (RIXS). Sharp peaks corresponding to the excitations of dimer orbitals are observed and analyzed by a combination of density functional theory (DFT) calculations and theoretical simulations based on a Ir-Ir cluster model. Such partially delocalized dimer states lead to a re-definition of the angular momentum of the electrons and changes in the magnetic and electronic behaviors of the material. We use this to explain the reduction of the observed magnetic moment with respect to prediction based on atomic states. This study opens new directions to study dimerization in a large family of materials including solids, heterostructures, molecules and transient states.

cond-mat.str-el↗

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

Origin of magnetic excitation gap in double perovskite Sr$_2$FeOsO$_6$

Sr$_2$FeOsO$_6$ is an insulating double perovskite compound which undergoes antiferromagnetic transitions at 140 K ($T_{N1}$) and 67 K ($T_{N2}$). To study the underlying electronic and magnetic interactions giving rise to this behavior we have performed inelastic neutron scattering (INS) and resonant inelastic x-ray scattering (RIXS) experiments on polycrystalline samples of Sr$_2$FeOsO$_6$. The INS data reveal that the spectrum of spin excitations remains ungapped below T$_{N1}$, however below T$_{N2}$ a gap of 6.8 meV develops. The RIXS data reveals splitting of the T$_{2g}$ multiplet consistent with that seen in other 5d$^3$ osmium based double perovskites. Together these results suggest that spin-orbit coupling is important for ground state selection in 3d-5d$^3$ double perovskite materials.

cond-mat.str-el↗