arXiv subjects

H. Gretarsson

Publications and source records attributed to H. Gretarsson.

At least 19 recordsLinked to original sources

arXiv2026

Between Mott and cluster Mott: spin-orbit entangled dimer singlets in Ba$_3$CeRu$_2$O$_9$

The hexagonal 4d ruthenates Ba3MRu2O9 host structural dimers and exhibit a delicate balance of competing interactions. Hund's coupling, trigonal crystal-field splitting, and hopping for $a_{1g}$ and $e_g^π$ orbitals all fall within a narrow energy window. This yields a series of possible ground states, ranging from the localized Mott limit with (anti-) ferromagnetic exchange coupling via orbital-selective behavior to the cluster Mott limit with quasimolecular orbitals that are delocalized over the two dimer sites. Using resonant inelastic x-ray scattering, we show that Ba3CeRu2O9 with four holes per dimer resides in the intricate crossover regime between the localized Mott case and the quasimolecular limit. The spin-orbit entangled singlet ground state predominantly shows a Mott-like charge distribution with two holes per Ru site. At the same time, spin and orbital occupation contradict an exchange-based Mott scenario but agree with a cluster Mott approach. A quasimolecular trial wave function describes more than 70% of the ground state. In this crossover regime, small changes of, e.g., the crystal field may strongly affect the character of electronic states.

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arXiv2026

Three-dimensional zigzag correlations in the van der Waals Kitaev magnet RuBr$_3$

Ruthenium trihalides Ru$X_3$ ($X$ = Cl, Br, I) provide a tunable platform for Kitaev magnetism in two-dimensional van der Waals materials. Despite their similar crystal structures and zigzag antiferromagnetic order, RuBr$_3$ exhibits a higher Néel temperature ($T_N$) than RuCl$_3$, suggesting their distinct proximity to the Kitaev quantum spin liquid phase. Using Ru $L_3$-edge resonant x-ray scattering, we show that, while the long-range zigzag order in RuBr$_3$ disappears at $T_N$, the zigzag correlations that persist well above $T_N$ show a pronounced spectral weight redistribution along the interlayer direction. These results suggest that the enhanced interlayer magnetic interactions driven by the extended Br 4$p$ orbitals stabilize three-dimensional zigzag correlations in RuBr$_3$.

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arXiv2025

Magnetic ground state of the dimer-based hexagonal perovskite Ba$_{3}$ZnRu$_{2}$O$_{9}$

We investigate the magnetic ground state of single crystals of the ruthenium-dimer-based hexagonal perovskite Ba$_{3}$ZnRu$_{2}$O$_{9}$ using magnetic susceptibility and resonant inelastic x-ray scattering (RIXS) measurements. While a previous study on powder samples exhibited intriguing magnetic behavior, questions about whether the spin state within a Ru$_{2}$O$_{9}$ dimer is a conventional $S = 3/2$ dimer or an orbital-selective $S = 1$ dimer were raised. The RIXS spectra reveal magnetic excitations from Hund's intraionic multiplet and intradimer spin-triplet transitions. The observed transition energies of the Hund's intraionic multiplets align with the $S=3/2$ ground state, contrasting with the theoretically proposed orbital-selective $S=1$ dimer state. High-temperature magnetic susceptibility analysis confirms the realization of the spin $S=3/2$ dimer state, and the extracted intradimer coupling is consistent with the spin-triplet transition energy observed in the RIXS spectra. These results highlights the ability of "spectroscopic fingerprinting" by RIXS to determine the magnetic ground states of complex materials.

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arXiv2024

$J=1/2$ Pseudospins and $d$-$p$ Hybridization in the Kitaev Spin Liquid Candidates Ru$X_3$ ($X$ = Cl, Br, I)

The recent synthesis of ruthenium trihalides Ru$X_3$ ($X$ = Cl, Br, I) has enlarged the set of material candidates for Kitaev spin liquid. The realization of Kitaev model necessitates the formation of $J=1/2$ pseudospins in the octahedral crystal field. We use Ru $L_3$-edge resonant inelastic x-ray scattering to investigate the evolution of multiplet structures in Ru$X_3$. We identified quasi-elastic magnetic correlations and spin-orbit transitions to the $J=3/2$ states without discernible trigonal splitting, thereby validating the $J=1/2$ description of magnetism in the Ru$X_3$ family. Lineshape broadening in RuI$_3$ provides evidence for its bulk metallicity in the vicinity of a bandwidth-controlled metal-insulator transition. Our results highlight the pivotal role of halogen $p$ orbitals in controlling the electronic properties of Ru$X_3$.

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arXiv2022

Distinct spin and orbital dynamics in Sr$_{2}$RuO$_{4}$

The unconventional superconductor Sr$_2$RuO$_4$ has long served as a benchmark for theories of correlated-electron materials. The determination of the superconducting pairing mechanism requires detailed experimental information on collective bosonic excitations as potential mediators of Cooper pairing. We have used Ru $L_3$-edge resonant inelastic x-ray scattering to obtain comprehensive maps of the electronic excitations of Sr$_2$RuO$_4$ over the entire Brillouin zone. We observe multiple branches of dispersive spin and orbital excitations associated with distinctly different energy scales. The spin and orbital dynamical response functions calculated within the dynamical mean-field theory are in excellent agreement with the experimental data. Our results highlight the Hund metal nature of Sr$_{2}$RuO$_{4}$ and provide key information for the understanding of its unconventional superconductivity.

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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.

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arXiv2021

Formation of orbital molecules on a pyrochlore lattice induced by A-O bond covalency

The pyrochlore ruthenate In$_2$Ru$_2$O$_7$ displays a subtle competition between spin-orbital entanglement and molecular orbital formation. At room temperature, a spin-orbit-entangled singlet state was identified. With decreasing temperature, In$_2$Ru$_2$O$_7$ undergoes multiple structural transitions and eventually forms a nonmagnetic ground state with semi-isolated Ru$_2$O units on the pyrochlore lattice. The dominant hopping through the Ru-O-Ru linkage leads to molecular orbital formation within the Ru$_2$O units. This molecular orbital formation is unique in that it involves the O$^{2-}$ anions, unlike the transition-metal dimers observed in systems with edge-sharing octahedra. We argue that the covalent character of In-O bonds plays a pivotal role in the structural transitions and molecular orbital formation and such bonding character of "$A$-site" ions is an important ingredient for electronic phase competition in complex transition metal oxides.

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arXiv2021

Absence of temperature-dependent phonon anomalies in Sr2IrO4 and Sr3Ir2O7

Following previous works reporting an anomalous behavior of several zone-center optical phonons across the magnetic transition of square lattice iridates Sr2IrO4 and Sr3Ir2O7, we have investigated the lattice dynamics as a function of momentum in these materials by means of high-resolution inelastic x-ray scattering (IXS). The observed phonon energies and scattering intensities across the Brillouin zone are in excellent agreement with ab-initio lattice dynamical calculations based on non-magnetic density-functional-perturbation theory (DFPT). Our results do not evidence any renormalization of the phonons at finite momentum across the magnetic transition of Sr2IrO4. The only anomalous behavior was detected for the in-plane polarized longitudinal-acoustic phonon branch in Sr3Ir2O7, which anomalously softens towards low temperatures and might be related to anisotropic negative thermal expansion in this compound. No anomalies related to potential charge ordering were observed.

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arXiv2021

Nonmagnetic $J = 0$ State and Spin-Orbit Excitations in K$_{2}$RuCl$_{6}$

Spin-orbit Mott insulators composed of $t_{2g}^4$ transition metal ions may host excitonic magnetism due to the condensation of spin-orbital $J=1$ triplons. Prior experiments suggest that the $4d$ antiferromagnet Ca$_{2}$RuO$_{4}$ embodies this notion, but a $J = 0$ nonmagnetic state as a basis of the excitonic picture remains to be confirmed. We use Ru $L_3$-edge resonant inelastic x-ray scattering to reveal archetypal $J$ multiplets with a $J=0$ ground state in the cubic compound K$_{2}$RuCl$_{6}$, which are well described within the $LS$-coupling scheme. This result highlights the critical role of unquenched orbital moments in $4d$-electron compounds and calls for investigations of quantum criticality and excitonic magnetism on various crystal lattices.

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arXiv2021

Selective orbital imaging of excited states with x-ray spectroscopy: the example of $α$-MnS

Herein we show that non-resonant inelastic x-ray scattering involving an $s$ core level is a powerful spectroscopic method to characterize the excited states of transition metal compounds. The spherical charge distribution of the $s$ core hole allows the orientational dependence of the intensities of the various spectral features to produce a spatial charge image of the associated multiplet states in a straightforward manner, thereby facilitating the identification of their orbital character. In addition, the $s$ core hole does not add an extra orbital angular momentum component to the multiplet structure so that the well-established Sugano-Tanabe-Kamimura diagrams can be used for the analysis of the spectra. For $α$-MnS we observe the spherical charge density corresponding to its high spin $3d^5$ ($^6A_1$) ground state configuration and we were able to selectively image its excited states and identify them as $t_{2g}$ ($^5T_2$) and $e_g$ ($^5E$) with an energy splitting $10Dq$ of 0.78\,eV.

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arXiv2020

Proximate ferromagnetic state in the Kitaev model material $α$-RuCl$_{3}$

$α$-RuCl$_{3}$ is a major candidate for the realization of the Kitaev quantum spin liquid, but its zigzag antiferromagnetic order at low temperatures indicates deviations from the Kitaev model. We have quantified the spin Hamiltonian of $α$-RuCl$_{3}$ by a resonant inelastic x-ray scattering study at the Ru $L_{3}$ absorption edge. In the paramagnetic state, the quasi-elastic intensity of magnetic excitations has a broad maximum around the zone center without any local maxima at the zigzag magnetic Bragg wavevectors. This finding implies that the zigzag order is fragile and readily destabilized by competing ferromagnetic correlations. The classical ground state of the experimentally determined Hamiltonian is actually ferromagnetic. The zigzag state is stabilized via a quantum "order by disorder" mechanism, leaving ferromagnetism -- along with the Kitaev spin liquid -- as energetically proximate metastable states. The three closely competing states and their collective excitations hold the key to the theoretical understanding of the unusual properties of $α$-RuCl$_{3}$ in magnetic fields.

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arXiv2020

Spin and charge excitations in the correlated multiband metal Ca3Ru2O7

We use Ru $L_3$-edge resonant inelastic x-ray scattering (RIXS) to study the full range of excitations in Ca$_3$Ru$_2$O$_7$ from meV-scale magnetic dynamics through to the eV-scale interband transitions. This bilayer $4d$-electron correlated metal expresses a rich phase diagram, displaying long range magnetic order below 56 K followed by a concomitant structural, magnetic and electronic transition at 48 K. In the low temperature phase we observe a magnetic excitation with a bandwidth of $\sim$30 meV and a gap of $\sim$8 meV at the zone center, in excellent agreement with inelastic neutron scattering data. The dispersion can be modeled using a Heisenberg Hamiltonian for a bilayer $\mathrm{S}=1$ system with single ion anisotropy terms. At a higher energy loss, $dd$-type excitations show heavy damping in the presence of itinerant electrons, giving rise to a fluorescence-like signal appearing between the $t_{2g}$ and $e_g$ bands. At the same time, we observe a resonance originating from localized $t_{2g}$ excitations, in analogy to the structurally related Mott-insulator Ca$_2$RuO$_4$. But whereas Ca$_2$RuO$_4$ shows sharp separate spin-orbit excitations and Hund's-rule driven spin-state transitions, here we identify only a single broad asymmetric feature. These results indicate that local intra-ionic interactions underlie the correlated physics in Ca$_3$Ru$_2$O$_7$, even as the excitations become strongly mixed in the presence of itinerant electrons.

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arXiv2019

Hidden structural transition in epitaxial Ca$_{0.5}$Sr$_{0.5}$IrO$_{3}$/SrTiO$_{3}$ thin film

A structural transition in an ABO$_{3}$ perovskite thin film involving the change of the BO$_{6}$ octahedral rotation pattern can be hidden under the global lattice symmetry imposed by the substrate and often easily overlooked. We carried out high-resolution x-ray diffraction experiments to investigate the structures of epitaxial Ca$_{0.5}$Sr$_{0.5}$IrO$_{3}$ (CSIO) perovskite iridate films grown on the SrTiO$_{3}$ (STO) and GdScO$_{3}$ (GSO) substrates in detail. Although the CSIO/STO film layer displays a global tetragonal lattice symmetry evidenced by the reciprocal space mapping, synchrotron x-ray data indicates that its room temperature structure is monoclinic due to Glazer's a$^{+}$a$^{-}$c$^{-}$-type rotation of the IrO$_{6}$ octahedra. In order to accommodate the lower-symmetry structure under the global tetragonal symmetry, the film breaks into four twinned domains, resulting in the splitting of the (half-integer, 0, integer) superlattice reflections. Surprisingly, the splitting of these superlattice reflections decrease with increasing temperature, eventually disappearing at T$_{S}$ = 510(5) K, which signals a structural transition to an orthorhombic phase with a$^{+}$a$^{-}$c$^{0}$ octahedral rotation. In contrast, the CSIO/GSO film displays a stable monoclinic symmetry with a$^{+}$b$^{-}$c$^{-}$ octahedral rotation, showing no structural instability caused by the substrate up to 520 K. Our study illustrates the importance of the symmetry in addition to the lattice mismatch of the substrate in determining the structure of epitaxial thin films.

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arXiv2019

Compressive-strain induced enhancement of exchange interactions and short-range magnetic order in Sr$_2$IrO$_4$ investigated by Raman spectroscopy

We have carried out Raman spectroscopy experiments to investigate two-magnon excitations in epitaxial thin films of the quasi-two-dimensional antiferromagnetic Mott insulator Sr$_2$IrO$_4$ under in-plane misfit strain. With in-plane biaxial compression, the energy of the two-magnon peak increases, and the peak remains observable over a wider temperature range above the Néel temperature, indicating strain-induced enhancement of the superexchange interactions between $\it{J}_{eff}$ = 1/2 pseudospins. From density functional theory calculations, we have found an increase of the nearest-neighbor hopping parameter and exchange interaction with increasing biaxial compressive strain, in agreement with the experimental observations. Our experimental and theoretical results provide perspectives for systematic, theory-guided strain control of the primary exchange interactions in 5$\it{d}$ transition metal oxides.

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arXiv2019

Orientation of ground-state orbital in CeCoIn$_5$ and CeRhIn$_5$

We present core level non-resonant inelastic x-ray scattering (NIXS) data of the heavy fermion compounds CeCoIn$_5$ and CeRhIn$_5$ measured at the Ce $N_{4,5}$-edges. The higher than dipole transitions in NIXS allow determining the orientation of the $Γ_7$ crystal-field ground-state orbital within the unit cell. The crystal-field parameters of the Ce$M$In$_5$ compounds and related substitution phase diagrams have been investigated in great detail in the past; however, whether the ground-state wavefunction is the $Γ_7^+$ ($x^2\,-\,y^2$) or $Γ_7^-$ ($xy$ orientation) remained undetermined. We show that the $Γ_7^-$ doublet with lobes along the (110) direction forms the ground state in CeCoIn$_5$ and CeRhIn$_5$. For CeCoIn$_5$, however, we find also some contribution of the first excited state crystal-field state in the ground state due to the stronger hybridization of 4$f$ and conduction electrons, suggesting a smaller $α^2$ value than originally anticipated from x-ray absorption. A comparison is made to the results of existing density functional theory plus dynamical mean-field theory calculations.

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arXiv2019

Observation of spin-orbit excitations and Hund's multiplets in Ca$_2$RuO$_4$

We use Ru $L_3$-edge (2838.5 eV) resonant inelastic x-ray scattering (RIXS) to quantify the electronic structure of Ca$_2$RuO$_4$, a layered $4d$-electron compound that exhibits a correlation-driven metal-insulator transition and unconventional antiferromagnetism. We observe a series of Ru intra-ionic transitions whose energies and intensities are well described by model calculations. In particular, we find a $\rm{J}=0\rightarrow 2$ spin-orbit excitation at 320 meV, as well as Hund's-rule driven $\rm{S}=1\rightarrow 0$ spin-state transitions at 750 and 1000 meV. The energy of these three features uniquely determines the spin-orbit coupling, tetragonal crystal-field energy, and Hund's rule interaction. The parameters inferred from the RIXS spectra are in excellent agreement with the picture of excitonic magnetism that has been devised to explain the collective modes of the antiferromagnetic state. $L_3$-edge RIXS of Ru compounds and other $4d$-electron materials thus enables direct measurements of interactions parameters that are essential for realistic model calculations.

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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.

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arXiv2019

Spin waves and spin-state transitions in a ruthenate high-temperature antiferromagnet

Ruthenium compounds play prominent roles in materials research ranging from oxide electronics to catalysis, and serve as a platform for fundamental concepts such as spin-triplet superconductivity, Kitaev spin-liquids, and solid-state analogues of the Higgs mode in particle physics. However, basic questions about the electronic structure of ruthenates remain unanswered, because several key parameters (including the Hund's-rule, spin-orbit, and exchange interactions) are comparable in magnitude, and their interplay is poorly understood - partly due to difficulties in synthesizing sizable single crystals for spectroscopic experiments. Here we introduce a resonant inelastic x-ray scattering (RIXS) technique capable of probing collective modes in microcrystals of $4d$-electron materials. We present a comprehensive set of data on spin waves and spin-state transitions in the honeycomb antiferromagnet SrRu$_{2}$O$_{6}$, which possesses an unusually high Néel temperature. The new RIXS method provides fresh insight into the unconventional magnetism of SrRu$_{2}$O$_{6}$, and enables momentum-resolved spectroscopy of a large class of $4d$ transition-metal compounds.

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