arXiv subjects

Diego Casa

Publications and source records attributed to Diego Casa.

16 recordsLinked to original sources

arXiv2026

Witnessing Quantum Entanglement Using Resonant Inelastic X-ray Scattering

Although entanglement is both a central ingredient in our understanding of quantum many-body systems and an essential resource for quantum technologies, we only have a limited ability to quantify entanglement in real quantum materials. Thus far, entanglement metrology in quantum materials has been limited to measurements involving Hermitian operators, such as the detection of spin entanglement using inelastic neutron scattering. Here, we devise a method to extract the quantum Fisher information (QFI) from non-Hermitian operators and formulate an entanglement witness for resonant inelastic x-ray scattering (RIXS). Our approach is then applied to the model iridate dimer system Ba$_3$CeIr$_2$O$_9$ and used to directly test for entanglement of the electronic orbitals between neighboring Ir sites. We find the entanglement can be detected if we account for the expected symmetries, parity, and electron number conservation, of the dimer system. We also consider the roles that the incident and outgoing x-ray polarizations and the incident photon energy play in entanglement detection. Our protocol provides a new handle for entanglement detection in quantum materials.

cond-mat.str-el↗

arXiv2023

Low-energy electronic interactions in ferrimagnetic Sr2CrReO6 thin films

We reveal in this study the fundamental low-energy landscape in the ferrimagnetic Sr2CrReO6 double perovskite and describe the underlying mechanisms responsible for the three low-energy excitations below 1.4 eV. Based on resonant inelastic x-ray scattering and magnetic dynamics calculations, and experiments collected from both Sr2CrReO6 powders and epitaxially strained thin films, we reveal a strong competition between spin-orbit coupling, Hund's coupling, and the strain-induced tetragonal crystal field. We also demonstrate that a spin-flip process is at the origin of the lowest excitation at 200 meV, and we bring insights into the predicted presence of orbital ordering in this material. We study the nature of the magnons through a combination of ab initio and spin-wave theory calculations, and show that two nondegenerate magnon bands exist and are dominated either by rhenium or chromium spins. The rhenium band is found to be flat at about 200 meV ($\pm$25 meV) through X-L-W-U high-symmetry points and is dispersive toward $Γ$

cond-mat.str-el↗

arXiv2023

Non-local features of the spin-orbit exciton in Kitaev materials

A comparative resonant inelastic x-ray scattering (RIXS) study of three well-known Kitaev materials is presented: $α$-Li$_2$IrO$_3$, Na$_2$IrO$_3$, and $α$-RuCl$_3$. Despite similar low-energy physics, these materials show distinct electronic properties, such as the large difference in the size of the charge gap. The RIXS spectra of the spin-orbit exciton for these materials show remarkably similar three-peak features, including sharp low energy peak (peak A) as well as transitions between $j_{\text{eff}}=1/2$ and $j_{\text{eff}}=3/2$ states. Comparison of experimental spectra with cluster calculations reveals that the observed three-peak structure reflects the significant role that non-local physics plays in the electronic structure of these materials. In particular, the low-energy peak A arises from a holon-doublon pair rather than a conventional particle-hole exciton as proposed earlier. Our study suggests that while spin-orbit assisted Mott insulator is still the best description for these materials, electron itinerancy cannot be ignored when formulating low-energy Hamiltonian of these materials.

cond-mat.str-el↗

arXiv2022

Interplay of broken symmetry and delocalized excitations in the insulating state of 1$T$-TaS$_2$

Coexistence of localized and extended excitations is central to the macroscopic properties of correlated materials. For 5d transition metal compounds, electron correlations alone generally do not lead to a metal-insulator (Mott) transition, with insulating behavior usually resulting from their coupling with magnetic ordering and/or structural distortions. 1$T$-TaS$_2$ is a prototypical example of such correlated insulating behavior, with a high-symmetry metallic phase transforming into a distorted, charge density wave (CDW) insulating state at low temperatures. The relevance of the localized electron physics at play in 3d compounds to these 5d transition metal compounds remains an open question. We resolved this standing controversy in 1$T$-TaS$_2$ combining resonant inelastic X-ray spectroscopy and first-principles calculations. We observed five electronic excitations arising from the interband transitions of the Ta 5d orbitals and the S 3p ligand state, with none of the excitations on the order of the Mott gap. These excitations cannot be explained within the framework of standard multiplet calculations that assume a localized wavefunction, but instead, are captured by a band theory framework accounting for the low symmetry of the crystal field in the CDW state. Our findings suggest that the electronic property of 1$T$-TaS$_2$ is dominated by both plasmonic quasiparticles and inter-band transitions associated with a Drude-type response, with no resonance associated with a putative Mott transition. Our discovery provides new insights into the electron localization and the onset of insulating behavior in 5d transition metal materials.

cond-mat.mtrl-sci↗

arXiv2022

Magnetic excitations in double perovskite iridates La$_{2}$$\mathit{M}$IrO$_{6}$ ($\mathit{M}$ = Co, Ni, and Zn) mediated by 3$\mathit{d}$-5$\mathit{d}$ hybridization

By performing resonant inelastic x-ray scattering (RIXS) measurements at the Ir $\mathit{L_{\mathrm{3}}}$ edge, we have investigated the low-energy elementary excitations in a series of double perovskite iridate single crystals, La$_{2}$$\mathit{M}$IrO$_{6}$ ($\mathit{M}$ = Co, Ni, and Zn). Almost dispersionless magnetic excitations at $\sim$ 42(6) meV and $\sim$ 35(5) meV have been observed in crystals containing magnetic 3$\mathit{d}$ ions, La$_{2}$CoIrO$_{6}$ and La$_{2}$NiIrO$_{6}$, respectively. In contrast, this low-energy magnetic excitation is absent in La$_{2}$ZnIrO$_{6}$ in which the 3$\mathit{d}$ ions are non-magnetic, suggesting the importance of 3$\mathit{d}$-5$\mathit{d}$ hybridization in the magnetic properties of these double perovskite iridates. The magnetic excitation is suppressed completely above the magnetic ordering temperature, suggesting the inadequacy of using a simple spin Hamiltonian to describe magnetism of these materials.

cond-mat.str-el↗

arXiv2021

Magnon-spinon dichotomy in the Kitaev hyperhoneycomb $β$-Li$_2$IrO$_3$

The family of edge-sharing tri-coordinated iridates and ruthenates has emerged in recent years as a major platform for Kitaev spin liquid physics, where spins fractionalize into emergent magnetic fluxes and Majorana fermions with Dirac-like dispersions. While such exotic states are usually pre-empted by long-range magnetic order at low temperatures, signatures of Majorana fermions with long coherent times have been predicted to manifest at intermediate and higher energy scales, similar to the observation of spinons in quasi-1D spin chains. Here we present a Resonant Inelastic X-ray Scattering study of the magnetic excitations of the hyperhoneycomb iridate $β$-Li$_2$IrO$_3$ under a magnetic field with a record-high-resolution spectrometer. At low-temperatures, dispersing spin waves can be resolved around the predicted intertwined incommensurate spiral and field-induced zigzag orders, whose excitation energy reaches a maximum of 16meV. A 2T magnetic field softens the dispersion around ${\bf Q}=0$. The behavior of the spin waves under magnetic field is consistent with our semiclassical calculations for the ground state and the dynamical spin structure factor, which further predicts that the ensued intertwined uniform states remain robust up to very high fields (100 T). Most saliently, the low-energy magnon-like mode is superimposed by a broad continuum of excitations, centered around 35meV and extending up to 100meV. This high-energy continuum survives up to at least 300K -- well above the ordering temperature of 38K -- and gives evidence for pairs of long-lived Majorana fermions of the proximate Kitaev spin liquid.

cond-mat.str-el↗

arXiv2020

Strain-engineering of the charge and spin-orbital interactions in Sr2IrO4

In the high spin-orbit coupled Sr2IrO4, the high sensitivity of the ground state to the details of the local lattice structure shows a large potential for the manipulation of the functional properties by inducing local lattice distortions. We use epitaxial strain to modify the Ir-O bond geometry in Sr2IrO4 and perform momentum-dependent Resonant Inelastic X-ray Scattering (RIXS) at the metal and at the ligand sites to unveil the response of the low energy elementary excitations. We observe that the pseudospin-wave dispersion for tensile-strained Sr2IrO4 films displays large softening along the [h,0] direction, while along the [h,h] direction it shows hardening. This evolution reveals a renormalization of the magnetic interactions caused by a strain-driven crossover from anisotropic to isotropic interactions between the magnetic moments. Moreover, we detect dispersive electron-hole pair excitations which shift to lower (higher) energies upon compressive (tensile) strain, manifesting a reduction (increase) in the size of the charge gap. This behavior shows an intimate coupling between charge excitations and lattice distortions in Sr2IrO4, originating from the modified hopping elements between the t2g orbitals. Our work highlights the central role played by the lattice degrees of freedom in determining both the pseudospin and charge excitations of Sr2IrO4 and provides valuable information towards the control of the ground state of complex oxides in the presence of high spin-orbit coupling.

cond-mat.str-el↗

arXiv2019

Exploring itinerant states in divalent hexaborides using rare-earth $L$ edge resonant inelastic X-ray scattering

We present a study of resonant inelastic X-ray scattering (RIXS) spectra collected at the rare-earth $L$ edges of divalent hexaborides YbB$_6$ and EuB$_6$. In both systems, RIXS-active features are observed at two distinct resonances separated by $\sim10$ eV in incident energy, with angle-dependence suggestive of distinct photon scattering processes. RIXS spectra collected at the divalent absorption peak strongly resemble the unoccupied 5$d$ density of states calculated using density functional theory, an occurrence we ascribe to transitions between weakly-dispersing 4$f$ and strongly dispersing 5$d$ states. In addition, anomalous resonant scattering is observed at higher incident energy, where no corresponding absorption feature is present. Our results suggest the far-reaching utility of $L$-edge RIXS in determining the itinerant-state properties of $f$-electron materials.

cond-mat.str-el↗

arXiv2018

Spin-orbit coupled systems in the "atomic" limit: rhenates, osmates, iridates

Motivated by RIXS experiments on a wide range of complex heavy oxides, including rhenates, osmates, and iridates, we discuss the theory of RIXS for site-localized $t_{2g}$ orbital systems with strong spin-orbit coupling. For such systems, we present exact diagonalization results for the spectrum at different electron fillings, showing that it accesses "single-particle" and "multi-particle" excitations. This leads to a simple picture for the energies and intensities of the RIXS spectra in Mott insulators such as double perovskites which feature highly localized electrons, and yields estimates of the spin-orbit coupling and Hund's coupling in correlated $5d$ oxides. We present new higher resolution RIXS data at the Re-L$_3$ edge in Ba$_2$YReO$_6$ which finds a previously unresolved peak splitting, providing further confirmation of our theoretical predictions. Using ab initio electronic structure calculations on Ba$_2$${\cal M}$ReO$_6$ (with ${\cal M}$=Re, Os, Ir) we show that while the atomic limit yields a reasonable effective Hamiltonian description of the experimental observations, effects such as $t_{2g}$-$e_g$ interactions and hybridization with oxygen are important. Our ab initio estimate for the strength of the intersite exchange coupling shows that, compared to the osmates, the exchange is one or two orders of magnitude weaker in the rhenates and iridates, which may partly explain the suppression of long-range magnetic order in the latter compounds. As a way to interpolate between the site-localized picture and our electronic structure band calculations, we discuss the spin-orbital levels of the ${\cal M}$O$_6$ cluster. This suggests a possible role for non-dispersive intra-cluster excitons in Ba$_2$YIrO$_6$ which may lead to a weak breakdown of the atomic $J_{\rm eff}=0$ picture and to small magnetic moments.

cond-mat.str-el↗

arXiv2018

Evolution of Magnetic Excitations Across the Metal-Insulator Transition in a Pyrochlore Iridate Eu$_{2}$Ir$_{2}$O$_{7}$

We report Resonant Inelastic X-ray Scattering (RIXS) study of the magnetic excitation spectrum in a highly insulating Eu$_{2}$Ir$_{2}$O$_{7}$ single crystal that exhibits a metal-insulator transition at $T_{MI}$ = 111(7) K. A propagating magnon mode with 20 meV bandwidth and 28 meV magnon gap is found in the excitation spectrum at 7 K, which is expected in the all-in-all-out (AIAO) magnetically ordered state. This magnetic excitation exhibits substantial softening as temperature is raised towards $T_{MI}$, and turns into highly damped excitation in the paramagnetic phase. Remarkably, the softening occurs throughout the whole Brillouin zone including the zone boundary. This observation is inconsistent with magnon renormalization expected in a local moment system, and indicates that the strength of electron correlation in Eu$_{2}$Ir$_{2}$O$_{7}$ is only moderate, so that electron itinerancy should be taken into account in describing its magnetism.

cond-mat.str-el↗

arXiv2017

Direct experimental observation of the molecular Jeff=3/2 ground state in the lacunar spinel GaTa4Se8

Strong spin-orbit coupling lifts the degeneracy of t2g orbitals in 5d transition-metal systems, leaving a Kramers doublet and quartet with effective angular momentum of Jeff = 1/2 and 3/2, respectively. These spin-orbit entangled states can host exotic quantum phases such as topological Mott state, unconventional superconductivity, and quantum spin liquid. The lacunar spinel GaTa4Se8 was theoretically predicted to form the molecular Jeff = 3/2 ground state. Experimental verification of its existence is an important first step to exploring the consequences of the Jeff = 3/2 state. Here, we report direct experimental evidence of the Jeff = 3/2 state in GaTa4Se8 by means of excitation spectra of resonant inelastic x-rays scattering at the Ta L3 and L2 edges. We found that the excitations involving the Jeff = 1/2 molecular orbital were suppressed only at the Ta L2 edge, manifesting the realization of the molecular Jeff = 3/2 ground state in GaTa4Se8.

cond-mat.str-el↗

arXiv2016

Giant Spin Gap and Magnon Localization in the Disordered Heisenberg Antiferromagnet Sr2Ir1-xRuxO4

We study the evolution of magnetic excitations in the disordered two-dimensional antiferromagnet Sr2Ir1-xRuxO4. A gigantic magnetic gap greater than 40 meV opens at x = 0.27 and increases with Ru concentration, rendering the dispersive magnetic excitations in Sr2IrO4 almost momentum independent. Up to a Ru concentration of x = 0.77, both experiments and first-principles calculations show the Ir Jeff = 1/2 state remains intact. The magnetic gap arises from the local interaction anisotropy in the proximity of the Ru disorder. Under the coherent potential approximation, we reproduce the experimental magnetic excitations using the disordered Heisenberg antiferromagnetic model with suppressed next-nearest neighbor ferromagnetic coupling.

cond-mat.str-el↗

arXiv2016

Pressure-Induced Confined Metal from the Mott Insulator Sr3Ir2O7

The spin-orbit Mott insulator Sr3Ir2O7 provides a fascinating playground to explore insulator-metal transition driven by intertwined charge, spin, and lattice degrees of freedom. Here, we report high pressure electric resistance and resonant inelastic x ray scattering measurements on single crystal Sr3Ir2O7 up to 63 65 GPa at 300 K. The material becomes a confined metal at 59.5 GPa, showing metallicity in the ab plane but an insulating behavior along the c axis. Such an unusual phenomenon resembles the strange metal phase in cuprate superconductors. Since there is no sign of the collapse of spin orbit or Coulomb interactions in x-ray measurements, this novel insulator metal transition is potentially driven by a first-order structural change at nearby pressures. Our discovery points to a new approach for synthesizing functional materials.

cond-mat.str-el↗

arXiv2016

A reexamination of the effective fine structure constant of graphene, as measured in graphite

We present a refined and improved study of the influence of screening on the effective fine structure constant of graphene, $α^*$, as measured in graphite using inelastic x-ray scattering. This follow-up to our previous study [J. P. Reed, et al., Science 330, 805 (2010)] was carried out with two times better energy resolution, five times better momentum resolution, and improved experimental setup with lower background. We compare our results to RPA calculations and evaluate the relative importance of interlayer hopping, excitonic corrections, and screening from high energy excitations involving the $σ$ bands. We find that the static, limiting value of $α^*$ falls in the range 0.25 to 0.35, which is higher than our previous result of 0.14, but still below the value expected from RPA. We show the reduced value is not a consequence of interlayer hopping effects, which were ignored in our previous analysis, but of a combination of excitonic effects in the $π\rightarrow π^*$ particle-hole continuum, and background screening from the $σ$-bonded electrons. We find that $σ$-band screening is extremely strong at distances of the order of a few nm, and should be highly effective at screening out short-distance, Hubbard-like interactions in graphene, as well as other carbon allotropes.

cond-mat.str-el↗

arXiv2011

The electron many-body problem in graphene

We give a brief summary of the current status of the electron many-body problem in graphene. We claim that graphene has intrinsic dielectric properties which should dress the interactions among the quasiparticles, and may explain why the observation of electron-electron renormalization effects has been so elusive in the recent experiments. We argue that the strength of Coulomb interactions in graphene may be characterized by an effective fine structure constant given by $α^{\star}(\mathbf{k},ω)\equiv2.2/ε(\mathbf{k},ω)$, where $ε(\mathbf{k},ω)$ is the dynamical dielectric function. At long wavelengths, $α^{\star}(\mathbf{k},ω)$ appears to have its smallest value in the static regime, where $α^{\star}(\mathbf{k}\to0,0)\approx1/7$ according to recent inelastic x-ray measurements, and the largest value in the optical limit, where $α^{\star}(0,ω)\approx2.6$. We conclude that the strength of Coulomb interactions in graphene is not universal, but depends highly on the scale of the phenomenon of interest. We propose a prescription in order to reconcile different experiments.

cond-mat.str-el↗

arXiv2010

The effective fine structure constant of freestanding graphene measured in graphite

Electrons in graphene behave like Dirac fermions, permitting phenomena from high energy physics to be studied in a solid state setting. A key question is whether or not these Fermions are critically influenced by Coulomb correlations. We performed inelastic x-ray scattering experiments on crystals of graphite, and applied reconstruction algorithms to image the dynamical screening of charge in a freestanding, graphene sheet. We found that the polarizability of the Dirac fermions is amplified by excitonic effects, improving screening of interactions between quasiparticles. The strength of interactions is characterized by a scale-dependent, effective fine structure constant, α*(k,ω), whose value approaches α* ~ 1/7 at low energy and large distances. This value is substantially smaller than the nominal α= 2.2, suggesting that, on the whole, graphene is more weakly interacting than previously believed.

cond-mat.str-el↗