Spin-Orbit-Induced Orbital Excitations in Sr2RuO4 and Ca2RuO4: A Resonant Inelastic X-ray Scattering Study
C. G. Fatuzzo, M. Dantz, S. Fatale, P. Olalde-Velasco, N. E. Shaik, B. Dalla Piazza, S. Toth, J. Pelliciari, R. Fittipaldi, A. Vecchione, N. Kikugawa, J. S. Bro… 展开作者
C. G. Fatuzzo, M. Dantz, S. Fatale, P. Olalde-Velasco, N. E. Shaik, B. Dalla Piazza, S. Toth, J. Pelliciari, R. Fittipaldi, A. Vecchione, N. Kikugawa, J. S. Brooks, H. M. Rønnow, M. Grioni, Ch. Rüegg, T. Schmitt, J. Chang
High-resolution resonant inelastic X-ray scattering (RIXS) at the oxygen K-edge has been used to study the orbital excitations of Ca2RuO4 and Sr2RuO4. In combination with linear dichroism X-ray absorption spectroscopy, the ruthenium 4d-orbital occupation and excitations were probed through their hybridization with the oxygen p-orbitals. These results are described within a minimal model, taking into account crystal field splitting and a spin-orbit coupling λ_{so}=200~meV. The effects of spin-orbit interaction on the electronic structure and implications for the Mott and superconducting ground states of (Ca,Sr)2RuO4 are discussed.
We demonstrate the utility of point group representation theory for symmetry analysis in resonant inelastic x-ray scattering. From its polarization-dependence, we show that a 5 eV inelastic feature in Sr2CuO2Cl2 has pure B1g symmetry and assign it to a transition in the cell-perturbation calculations of Simon, et. al. [Phys. Rev. B., 54, R3780 (1996)]. We discuss how Raman selection rules are broken at nonzero momentum transfer and how this can also act as a probe of wave function symmetry.
We develop a formalism to study indirect resonant inelastic x-ray scattering (RIXS) in systems with itinerant electrons, accounting for the attraction between valence electrons and the positively-charged core hole exactly, and apply this formalism to the hole-doped cuprate superconductors. We focus on the relationship between RIXS lineshapes and band structure, including broken symmetries. We show that RIXS is capable of distinguishing between competing order parameters, establishing it as a useful probe of the pseudogap phase.
We report a Cu K-edge resonant inelastic x-ray scattering (RIXS) study of momentum-dependent charge excitations in Nd$_{2-x}$Ce$_x$CuO$_4$ ($x$ = 0.075 and 0.18). The peak position and width of the excitations coincide excellently with those observed in Cu L$_3$-edge RIXS. It demonstrates that the same charge excitations are observed at the two edges.
Ru M$_3$-edge resonant inelastic x-ray scattering (RIXS) measurements of RuCl$_3$ with 27 meV resolution reveals a spin-orbit exciton without noticeable splitting. We extract values for the spin-orbit coupling constant ($λ=154\pm2$ meV) and trigonal distortion field energy ($\left|Δ\right|<65$ meV) which support the $j_{\rm eff}=1/2$ nature of RuCl$_3$. We demonstrate the feasibility of M-edge RIXS for $4d$ systems, which allows ultra high-resolution RIXS of $4d$ systems until instrumentation for L-edge RIXS improves.
The scattering cross section of the resonant inelastic light scattering is represented as a correlation function in the Keldysh-Schwinger functional integral formalism. The functional integral approach enables us to compute the cross section in the Feynman diagram perturbation theory where many-body effects can be fully incorporated. This approach is applied to the one G-phonon Raman scattering of graphene, and the result is shown to agree with the one previously obtained by the conventional Fermi golden rule formula. Also, this approach is generalized to the systems in non-equilibrium conditi…
Phonons, the quantum mechanical representation of lattice vibrations, and their coupling to the electronic degrees of freedom are important for understanding thermal and electric properties of materials. For the first time, phonons have been measured using resonant inelastic x-ray scattering (RIXS) across the Cu K-edge in cupric oxide (CuO). Analyzing these spectra using an ultra-short core-hole lifetime approximation and exact diagonalization techniques, we can explain the essential inelastic features. The relative spectral intensities are related to the electron-phonon coupling strengths.
I present a tractable theory for the Resonant Inelastic X-ray Scattering (RIXS) spectral function of magnons. The low-energy transition operator is written as a product of local spin operators times fundamental x-ray absorption spectra. This leads to simple selection rules for the magnetic cross section. The scattering cross section linear (quadratic) in spin operators is proportional to the magnetic circular (linear) dichroic absorption. RIXS is a novel tool to measure magnetic quasi particles (magnons) and the incoherent spectral weight, as well as multiple magnons up to very high energy los…
Orbital degrees of freedom play a major role in the physics of many strongly correlated transition metal compounds. However, they are still very difficult to access experimentally, in particular by neutron scattering. We propose here how to reveal orbital occupancies of the system ground state by magnetic resonant inelastic x-ray scattering (RIXS). This is possible because, unlike in neutron scattering, the intensity of the magnetic excitations in RIXS depends essentially on the symmetry of the orbitals where the spins are in.
We develop a framework to evaluate the time-dependent resonant inelastic X-ray scattering (RIXS) signal with the use of non-equilibrium dynamical mean field theory simulations. The approach is based on the solution of a time-dependent impurity model which explicitly incorporates the probe pulse. It avoids the need to compute four-point correlation functions, and can in principle be combined with different impurity solvers. This opens a path to study time-resolved RIXS processes in multi-orbital systems. The approach is exemplified with a study of the RIXS signal of a melting Mott antiferromagn…
Predictions are made for the momentum- and carrier-dependent degradation of the Mott gap upon doping in high-Tc cuprates as would be observed in Cu K-edge resonant inelastic x-ray scattering (RIXS). The two-dimensional Hubbard model with second- and third-nearest-neighbor hopping terms has been studied by numerical exact diagonalization. Special emphasis is placed on the particle-hole asymmetry of the Mott gap excitations. We argue that the Mott gap excitations observed by RIXS are significantly influenced by the interaction between charge carriers and antiferromagnetic correlations.
We report resonant inelastic x-ray measurements of insulating La$_2$CuO$_4$ and Sr$_2$CuO$_2$Cl$_2$ taken with the incident energy tuned near the Cu K absorption edge. We show that the spectra are well described in a shakeup picture in 3rd order perturbation theory which exhibits both incoming and outgoing resonances, and demonstrate how to extract a spectral function from the raw data. We conclude by showing {\bf q}-dependent measurements of the charge transfer gap.
Effective symmetry-based transition operators for resonant inelastic X-ray scattering (RIXS) are derived that show how the scattering between different states depends on the polarization of the incoming and outgoing X-rays. In spherical symmetry, the effective operators can be rewritten in terms of spin operators, although the expressions depend on the nature of the ground state. For lower symmetries, the combined action of the crystal field and the spin-orbit interaction breaks up the spin space and spin operators are no longer appropiate operators. By taking iridium compounds as an example, …
We study theoretically the resonant inelastic x-ray scattering in quasi-one-dimensional insulating copper oxides, where the incident photon energy is tuned to the Cu1s-4p absorption energy. Our attention is focused particularly on the strong momentum-transfer dependence of the spectral shape observed in recent experiments. We describe the antiferromagnetic ground state within the Hartree-Fock theory, and consider charge excitations from the ground state within the random phase approximation. By taking account of the electron correlation effects perturbatively, we obtain detailed momentum-trans…
The recent discovery that resonant inelastic x-ray scattering can probe single-magnon (SM) dispersions in transition metal (TM) oxides when the x-ray energy is tuned to the TM $L$-edge, has put this technique on a par with inelastic neutron scattering. It is generally presumed that selection rules forbid SM-scattering at oxygen (O) $K$-edges. However, based on a symmetry analysis and exact diagonalization study, we show that SM-scattering at O K-edges becomes allowed when (i) spin-orbit coupling is present in the TM d-shell and (ii) inversion symmetry at the O-site is broken. For cuprates the …
We report strongly momentum-dependent local charge screening dynamics in CE-type charge, orbital, and spin ordered La$_{0.5}$Sr$_{1.5}$MnO$_4$, based on Mn K-edge resonant inelastic x-ray scattering data. Through a comparison with theoretical calculations, we show that the observed momentum dependence reflects highly localized, nearest neighbor screening of the transient local charge perturbation in this compound with an exciton-like screening cloud, rather than delocalized screening. The size of the screening cloud is estmated to be about 0.4-0.5 interatomic distances.
Resonant inelastic x-ray scattering (RIXS) at the oxygen $K$-edge has recently accessed multi-spinon excitations in the one-dimensional antiferromagnet (1D-AFM) \sco, where four-spinon excitations are resolved separately from the two-spinon continuum. This technique, therefore, provides new opportunities to study fractionalized quasiparticle excitations in doped 1D-AFMs. To this end, we carried out exact diagonalization studies of the doped $t$-$J$ model and provided predictions for oxygen $K$-edge RIXS experiments on doped 1D-AFMs. We show that the RIXS spectra are rich, containing distinct t…
Although orbital degrees of freedom are a factor of fundamental importance in strongly correlated transition metal compounds, orbital correlations and dynamics remain very difficult to access, in particular by neutron scattering. Via a direct calculation of scattering amplitudes we show that instead magnetic resonant inelastic x-ray scattering (RIXS) does reveal orbital correlations. In contrast to neutron scattering, the intensity of the magnetic excitations in RIXS depends very sensitively on both the symmetry of the orbitals that spins occupy, and on photon polarizations. We show in detail …
Recent experiments show that indirect resonant inelastic X-ray scattering (RIXS) is a new probe of spin dynamics. Here I derive the cross-section for magnetic RIXS and determine the momentum dependent four-spin correlation function that it measures. These results show that this technique offers information on spin dynamics that is complementary to e.g. neutron scattering. The RIXS spectrum of Heisenberg antiferromagnets is calculated. It turns out that only scattering processes that involve at least two magnons are allowed. Other selection rules imply that the scattering intensity vanishes for…
Element- and site-specific resonant inelastic x-ray scattering spectroscopy (RIXS) is employed to investigate electron correlation effects in {$\rm NaV_2O_5$}. In contrast to single photon techniques, RIXS at the vanadium $L_3$ edge is able to probe $d-d^*$ transitions between V d-bands. A sharp energy loss feature is observed at -1.56 eV, which is well reproduced by a model calculation including correlation effects. The calculation identifies the loss feature as excitation between the lower and upper Hubbard bands and permits an accurate determination of the Hubbard interaction term $U= 3.0 \…
We report a high-resolution resonant inelastic soft x-ray scattering study of the quantum magnetic spin-chain materials Li2CuO2 and CuGeO3. By tuning the incoming photon energy to the oxygen K-edge, a strong excitation around 3.5 eV energy loss is clearly resolved for both materials. Comparing the experimental data to many-body calculations, we identify this excitation as a Zhang-Rice singlet exciton on neighboring CuO4-plaquettes. We demonstrate that the strong temperature dependence of the inelastic scattering related to this high-energy exciton enables to probe short-range spin correlations…
We analyze resonant inelastic x-ray scattering (RIXS) at the Cu K edge in a typical orbital-ordered compound KCuF3 on the basis of a microscopic theory. Spectral shape and its dependence on polarization direction and momentum transfer of photons are explained consistently with experimental data within our microscopic calculation. According to our microscopic orbital-resolving analysis, high-energy spectral weights (above 5 eV) originate from charge-transfer excitations related to the Cu-dγorbitals, while the low-energy weights (below 2 eV) originate from the d-d orbital excitations among the f…
Using the three-orbital Hubbard model, we investigate the low-energy excitation spectra in the antiferromagnetic phase of Ca$_2$RuO$_4$. We calculate the dynamical susceptibilities in the low-energy region by the random phase approximation and find that the anisotropic dispersion of the transverse mode is in good agreement with the spectra recently reported by inelastic neutron scattering experiments. By the fast-collision approximation, we simulate the resonant inelastic x-ray scattering (RIXS) spectra of the Ru $L_3$ edge from the dynamical susceptibilities. We show that the dispersion of th…
We present a theoretical investigation of the origin of Raman-like and fluorescencelike (FL) features of resonant inelastic x-ray scattering (RIXS) spectra. Using a combination of local-density approximation + dynamical mean-field theory and a configuration interaction solver for Anderson impurity model, we calculate the $L$-edge RIXS and x-ray absorption spectra of high-valence transition-metal oxides LaCuO$_3$ and NaCuO$_2$. We analyze in detail the behavior of the FL feature and show how it is connected to the details of electronic and crystal structure. On the studied compounds we demonstr…
We provide a semiquantitative explanation of a recent experiment on the resonant inelastic x-ray scattering (RIXS) in insulating cuprate La2CuO4 (Y.J. Kim et al., Phys. Rev. Lett. 89, 177003 (2002).). We show theoretically that there are three characteristic peaks in RIXS spectra, two of which are attributed to the charge transfer excitation and are reasonably assigned to those observed experimentally. The lowest energy peak has a relatively large dispersion ($\sim 0.8$ eV) and is suppressed near the zone corner (π, π), in agreement with the experiment. We stress that electron correlation is a…
We calculate the resonant inelastic X-ray scattering (RIXS) response of the Kitaev honeycomb model, an exactly solvable quantum-spin-liquid model with fractionalized Majorana and flux excitations. We find that the fundamental RIXS channels, the spin-conserving (SC) and the non-spin-conserving (NSC) ones, do not interfere and give completely different responses. SC-RIXS picks up exclusively the Majorana sector with a pronounced momentum dispersion, whereas NSC-RIXS also creates immobile fluxes, thereby rendering the response only weakly momentum dependent, as in the spin structure factor measur…
We report the observation of temperature dependent electronic excitations in various manganites utilizing resonant inelastic x-ray scattering (RIXS) at the Mn K-edge. Excitations were observed between 1.5 and 16 eV with temperature dependence found as high as 10 eV. The change in spectral weight between 1.5 and 5 eV was found to be related to the magnetic order and independent of the conductivity. On the basis of LDA+U and Wannier function calculations, this dependence is associated with intersite d-d excitations. Finally, the connection between the RIXS cross-section and the loss function is …
Nonresonant inelastic x-ray scattering (NIXS) is a possible tool to detect charge excitations in electron systems. In addition, multipole transitions at high-momentum-transfer region open a new possibility to determine orbital-selective electronic excitations in multi-orbital itinerant 3d electron systems. As a theoretical example, we chose the antiferromagnetic state of iron arsenides and demonstrate that the orbital-selective excitations are detectable by choosing appropriate momentum transfer in NIXS. We propose that both NIXS and resonant inelastic x-ray scattering are complementary to eac…
We derive general expressions for resonant inelastic x-ray scattering (RIXS) operators for $t_{2g}$ orbital systems, which exhibit a rich array of unconventional magnetism arising from unquenched orbital moments. Within the fast collision approximation, which is valid especially for 4$d$ and 5$d$ transition metal compounds with short core-hole lifetimes, the RIXS operators are expressed in terms of total spin and orbital angular momenta of the constituent ions. We then map these operators onto pseudospins that represent spin-orbit entangled magnetic moments in systems with strong spin-orbit co…
We investigate magnetic excitations in the spin-ladder compound Sr$_{14}$Cu$_{24}$O$_{41}$ using high-resolution Cu $L_3$-edge Resonant Inelastic X-ray Scattering (RIXS). Our findings demonstrate that RIXS couples to collective spin excitations from a quantum spin-liquid ground state. In contrast to Inelastic Neutron Scattering (INS), the RIXS cross section changes only moderately over the entire Brillouin Zone (BZ), revealing a high sensitivity also at small momentum transfers. The two-triplon energy gap is found to be $100\pm 30$ meV. Our results are supported by calculations within an effec…
We report a Cu K-edge resonant inelastic x-ray scattering (RIXS) study of orbital excitations in KCuF3 . By performing the polarization analysis of the scattered photons, we disclose that the excitation between the eg orbitals and the excitations from t2g to eg exhibit distinct polarization dependence. The polarization dependence of the respective excitations is interpreted based on a phenomenological consideration of the symmetry of the RIXS process that yields a necessary condition for observing the excitations. In addition, we show that the orbital excitations are dispersionless within our …
We present a study of the resonant inelastic scattering response of \ybin\ excited at the tender Yb $M_5$ X-ray edge. In the high-temperature, paramagnetic phase, we observe a multiplet structure which can be understood at an ionic level. Upon cooling through the valence transition at $T_v\sim$ 40$K$, we observe a strong renormalization of the low-energy spectra, indicating a sensitivity to the formation of an intermediate valence phase at low temperatures. Similar spectrum renormalization has been observed in the optical conductivity, which suggests that the low-energy electronic structure po…
Ruddlesden-Popper and reduced Ruddlesden-Popper nickelates are intriguing candidates for mimicking the properties of high-temperature superconducting cuprates. The degree of similarity between these nickelates and cuprates has been the subject of considerable debate. Resonant inelastic x-ray scattering (RIXS) has played an important role in exploring their electronic and magnetic excitations, but these efforts have been stymied by inconsistencies between different samples and the lack of publicly available data for detailed comparison. To address this issue, we present open RIXS data on La4Ni3…
We establish the spectral line shape of orbital excitations created by resonant inelastic X-ray scattering for the model Mott insulator CoO. Improved experimental energy resolution reveals that the line shapes are strikingly different from expectations in a first principles-based atomic multiplet model. Extended theoretical simulations are performed to identify the underlying physical origins, which include a pronounced thermal tail reminiscent of anti-Stokes scattering on the energy gain side of excitations, and an essential contribution from interatomic many-body dynamics on the energy loss …
Collective excitations contain rich information about photoinduced transient states in correlated systems. In a Mott insulator, charge degrees of freedom are frozen, but can be activated by photodoping. The energy-momentum distribution of the charge excitation spectrum reflects the propagation of charge degrees of freedom, and provides information about the interplay among various intertwined instabilities on the time scale set by the pump. To reveal charge excitations out of equilibrium, we simulate time-resolved x-ray absorption and resonant inelastic x-ray scattering using a Hubbard model. …
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 s…
We report empirical comparisons of Cu K-edge indirect resonant inelastic x-ray scattering (RIXS) spectra, taken at the Brillouin zone center, with optical dielectric loss functions measured in a number of copper oxides. The RIXS data are obtained for Bi$_2$CuO$_4$, CuGeO$_3$, Sr$_2$Cu$_3$O$_4$Cl$_2$, La$_2$CuO$_4$, and Sr$_2$CuO$_2$Cl$_2$, and analyzed by considering both incident and scattered photon resonances. An incident-energy-independent response function is then extracted. The dielectric loss functions, measured with spectroscopic ellipsometry, agree well with this RIXS response, especi…
We report on the most complete investigation to date of the 4f-electron properties at the gamma-alpha transition in elemental Ce by resonant inelastic x-ray scattering (RIXS). The Ce 2p3d-RIXS spectra were measured directly in the bulk material as a function of pressure through the transition. The spectra were simulated within the Anderson impurity model. The occupation number nf was derived from the calculations in both gamma- and alpha-phases in the ground state along with the f doubleoccupancy. We find that the electronic structure changes result mainly from band formation of 4f electrons w…
We report a resonant inelastic x-ray scattering study of the dispersion relations of charge transfer excitations in insulating La$_2$CuO$_4$. These data reveal two peaks, both of which show two-dimensional characteristics. The lowest energy excitation has a gap energy of $\sim 2.2$ eV at the zone center, and a dispersion of $\sim 1$ eV. The spectral weight of this mode becomes dramatically smaller around ($π$, $π$). The second peak shows a smaller dispersion ($\sim 0.5$ eV) with a zone-center energy of $\sim 3.9$ eV. We argue that these are both highly dispersive exciton modes damped by the pr…
More than 50 years ago the electron-hole attraction was proposed to drive narrow gap semiconductors or semimetals to a new phase, the excitonic insulator. The experimental proof of its existence in bulk materials remains elusive. In strongly correlated insulators, the proximity of the excitonic insulator phase is reflected by the presence of dispersive electron-hole excitations with a small gap above a singlet ground state. Recently, such an excitation spectrum was proposed to be realized in perovskite oxide LaCoO$_3$. In this Letter we use Co $L_3$-edge resonant inelastic X-ray scattering to …
We analyze theoretically the resonant inelastic x-ray scattering (RIXS) at the Ni K edge in the stripe-ordered state of La_{2-x}Sr_xNiO_4 at x=1/3. In the calculation of RIXS spectra, the stripe-ordered ground state is described within the Hartree-Fock approximation by using a realistic tight-binding model for Ni3dγand O2p_{x, y} orbitals, and the electron correlations in the electronic excitation processes are taken into account within the random-phase approximation. The calculated RIXS spectrum shows a tail toward the low-energy region when the momentum transfer of photons equals the stripe …
Momentum dependent charge excitations of a two-leg ladder are investigated by resonant inelastic x-ray scattering of (La,Sr,Ca)14Cu24O41. In contrast to the case of a square lattice, momentum dependence of the Mott gap excitation of the ladder exhibits little change upon hole-doping, indicating the formation of hole pairs. Theoretical calculation based on a Hubbard model qualitatively explains this feature. In addition, experimental data shows intraband excitation as continuum intensity below the Mott gap and it appears at all the momentum transfers simultaneously. The intensity of the intraba…
The community currently lacks a complete understanding of how resonant inelastic x-ray scattering (RIXS) experiments probe the electron-phonon ($e$-ph) interaction in solids. For example, most theoretical models of this process have focused on dispersionless Einstein phonons. Using a recently developed momentum average (MA) variational approximation for computing RIXS spectra of band insulators, we examine the influence of both electron and phonon dispersion in the intermediate state of the scattering process. We find that the inclusion of either, and their mutual interplay, introduces signifi…
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 dispersi…
We report a resonant inelastic x-ray scattering study of charge excitations in the quasi-one-dimensional Mott insulator SrCuO2. We observe a continuum of low-energy excitations, in which a highly dispersive feature with a large sinusoidal dispersion (~1.1 eV) resides. We have also measured the optical conductivity, and studied the dynamic response of the extended Hubbard model with realistic parameters, using a dynamical density-matrix renormalization group method. In contrast to earlier work, we do not find a long-lived exciton, but rather these results suggest that the excitation spectrum co…
We investigate electronic excitations in La2-x(Br,Sr)xCuO4 using resonant inelastic x-ray scattering (RIXS) at the oxygen K edge. RIXS spectra of the hole-doped cuprates show clear momentum dependence below 1 eV. The spectral weight exhibits positive dispersion and shifts to higher energy with increasing hole concentration. Theoretical calculation of the dynamical charge structure factor on oxygen orbitals in a three-band Hubbard model is consistent with the experimental observation of the momentum and doping dependence, and therefore the dispersive mode is ascribed to intraband charge excitat…
We theoretically investigate spin dynamics and $L_3$-edge resonant inelastic X-ray scattering (RIXS) of Chromium with commensurate spin-density wave (SDW) order, based on a multi-band Hubbard model composed of 3$d$ and 4$s$ orbitals. Obtaining the ground state with the SDW mean-field approximation, we calculate the dynamical transverse and longitudinal spin susceptibility by using random-phase approximation. We find that a collective spin-wave excitation seen in inelastic neutron scattering hardly damps up to $\sim$0.6 eV. Above the energy, the excitation overlaps individual particle-hole exci…
Vanadium dioxide is of broad interest as a spin-1/2 electron system that realizes a metal-insulator transition near room temperature, due to a combination of strongly correlated and itinerant electron physics. Here, resonant inelastic X-ray scattering is used to measure the excitation spectrum of charge, spin, and lattice degrees of freedom at the vanadium L-edge under different polarization and temperature conditions. These spectra reveal the evolution of energetics across the metal-insulator transition, including the low temperature appearance of a strong candidate for the singlet-triplet ex…
Generic low-energy spectral features related to $d$-$d$ excitations in nearly cubic vanadium perovskites are predicted for the expected $L$-edge resonant inelastic X-ray scattering (RIXS) measurements. Model Hamiltonian describing local electronic properties, including crystal-field effects, of vanadium 3d orbitals in the basic $t_{2g}^2$ configuration is formulated with the help of complementary {\it ab initio} quantum-chemical cluster calculations. In the presence of 2p-core hole, the local Hamiltonian includes strong 2p-3d electron interactions. As a prerequisite for evaluating RIXS transit…
We present a computation of Cu K-edge resonant inelastic x-ray scattering (RIXS) spectra for electron-doped cuprates which includes coupling to bosonic fluctuations. Comparison with experiment over a wide range of energy and momentum transfers allows us to identify the signatures of three key normal-state energy scales: the pseudogap, charge transfer gap, and Mott gap. The calculations involve a three band Hubbard Hamiltonian based on Cu $d_{x^2-y^2}$ and O $p_x$, $p_y$ orbitals, with a self-energy correction which arises due to spin and charge fluctuations. Our theory reproduces characteristi…
Young's archetypal double-slit experiment forms the basis for modern diffraction techniques: the elastic scattering of waves yields an interference pattern that captures the real-space structure. Here, we report on an inelastic incarnation of Young's experiment and demonstrate that resonant inelastic x-ray scattering (RIXS) measures interference patterns which reveal the symmetry and character of electronic excited states in the same way as elastic scattering does for the ground state. A prototypical example is provided by the quasi-molecular electronic structure of insulating Ba3CeIr2O9 with …
We examine the momentum-dependent excitation spectra of indirect as well as direct resonant inelastic x-ray scattering (RIXS) processes in half-filled (extended) Hubbard rings. We determine the fundamental features of the groundstate RIXS response and discuss the experimental conditions that can allow for the low-energy part of these features to be distinguished in one-dimensional copper-oxide materials, focusing particularly on the different magnetic excitations occurring in indirect and direct RIXS processes. We study the dependence of spin and charge excitations on the choice of and detunin…
We examine the effect of core-hole lifetime on the spectral weight of resonant inelastic x-ray scattering (RIXS) in hole-doped cuprates. We calculate the spectral weight by using exact diagonalization technique for a 4x4 doped Hubbard lattice and find that spin-flip channel detecting single-magnon excitation is less sensitive to the core-hole lifetime while in non-spin-flip channel the spectral weight is strongly dependent on the lifetime. In the latter, charge and two-magnon excitations predominately contribute to RIXS for short and long core-hole lifetimes, respectively. For a realistic valu…
We present a non-perturbative, divergence-free series expansion of Green's functions using effective operators. The method is especially suited for computing correlators of complex operators as a series of correlation functions of simpler forms. We apply the method to study low-energy excitations in resonant inelastic x-ray scattering (RIXS) in doped one- and two-dimensional single-band Hubbard models. The RIXS operator is expanded into polynomials of spin, density, and current operators weighted by fundamental x-ray spectral functions. These operators couple to different polarization channels…
We perform a comprehensive analysis of the bimagnon resonant inelastic x-ray scattering (RIXS) intensity spectra of the spatially frustrated Jx-Jy-J2 Heisenberg model on a square lattice in both the antiferromagnetic and the collinear antiferromagnetic phase. We study the model for strong frustration and significant spatial anisotropy to highlight the key signatures of RIXS spectrum splitting which may be experimentally discernible. Based on an interacting spin wave theory study within the ladder approximation Bethe-Salpeter scheme, we find the appearance of a robust two-peak structure over a …
We report resonant inelastic x-ray scattering experiments of the orbital ordered manganite LaMnO3. When the incident photon energy is tuned near the Mn K absorption edge, the spectra reveal three features at 2.5 eV, 8 eV and 11 eV. The 8 eV and 11 eV peaks are considered charge-transfer type excitations. On the other hand, theoretical calculations identify the 2.5 eV peak as an orbital excitation across the Mott gap, i.e. an electron excitation from the lower Hubbard band with the d3x2-r2 and d3y2-r2 orbital characters to the upper Hubbard band with the dy2-z2 and dz2-x2 ones. The observed wea…
Taking spinon excitations in the quantum antiferromagnet CaCu2O3 as an example, we demonstrate that femtosecond dynamics of magnetic excitations can be probed by direct resonant inelastic x-ray scattering (RIXS). To this end, we isolate the contributions of single and double spin-flip excitations in experimental RIXS spectra, identify the physical mechanisms that cause them and determine their respective timescales. By comparing theory and experiment, we find that double spin flips need a finite amount of time to be generated, rendering them sensitive to the core-hole lifetime, whereas single …
Electronic excitations near the Fermi energy in the hole doped manganese oxides (La1-xSrxMnO3, x=0.2 and 0.4) have been elucidated by using the resonant inelastic x-ray scattering (RIXS) method. A doping effect in the strongly correlated electron systems has been observed for the first time. The scattering spectra show that a salient peak appears in low energies indicating the persistence of the Mott gap. At the same time, the energy gap is partly filled by doping holes and the energy of the spectral weight shifts toward lower energies. The excitation spectra show little change in the momentum…
The resonant inelastic x-ray scattering (RIXS) was measured in an insulating SrCuO$_{2}$ with changing the incident photon energy ($hν$) near the Cu $1s$ absorption edge (K-edge). Complex structures and their dependences on the momentum transfer($Δk$) and $hν$ were observed. The $hν$ dependence of the RIXS spectra measured for a constant $Δk$=2.4$π$ has shown a remarkable enhancement near the absorption maximum and a shift of the spectral weight toward larger loss-energy with increasing $hν$. Also, the energy of the inelastic loss peak in the RIXS spectra for the fixed excitation at 8.993 keV,…
