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Register a new userSpin-Orbital Excitations in Ca$_{2}$RuO$_4$ Revealed by Resonant Inelastic X-ray Scattering
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The strongly correlated insulator Ca$_{2}$RuO$_4$ is considered as a paradigmatic realization of both spin-orbital physics and a band-Mott insulating phase, characterized by orbitally selective coexistence of a band and a Mott gap. We present a high-resolution oxygen $K$-edge resonant inelastic X-ray scattering study of the antiferromagnetic Mott insulating state of Ca$_{2}$RuO$_4$. A set of low-energy ($sim$80 and 400 meV) and high-energy ($sim$1.3 and 2.2 eV) excitations are reported that show strong incident light polarization dependence. Our results strongly support a spin-orbit coupled band-Mott scenario and explore in detail the nature of its exotic excitations. Guided by theoretical modelling, we interpret the low-energy excitations as a result of composite spin-orbital excitations. Their nature unveil the intricate interplay of crystal-field splitting and spin-orbit coupling in the band-Mott scenario. The high-energy excitations correspond to intra-atomic singlet-triplet transitions at an energy scale set by the Hunds coupling. Our findings give a unifying picture of the spin and orbital excitations in the band-Mott insulator Ca$_{2}$RuO$_4$.
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We present a combined oxygen $K$-egde x-ray absorption spectroscopy (XAS) and resonant inelastic x-ray scattering (RIXS) study of the bilayer ruthenate Ca$_3$Ru$_2$O$_7$. Our RIXS experiments on Ca$_3$Ru$_2$O$_7$ were carried out on the overlapping in-plane and inner apical oxygen resonances, which are distinguishable from the outer apical one. Comparison to equivalent oxygen $K$-edge spectra recorded on band-Mott insulating Ca$_2$RuO$_4$ is made. In contrast to Ca$_2$RuO$_4$ spectra, which contain excitations linked to Mott physics, Ca$_3$Ru$_2$O$_7$ spectra feature only intra-$t_{2g}$ ones that do not directly involve the Coulomb energy scale. As found in Ca$_2$RuO$_4$, we resolve two intra-$t_{2g}$ excitations in Ca$_3$Ru$_2$O$_7$. Moreover, the lowest lying excitation in Ca$_3$Ru$_2$O$_7$ shows a significant dispersion, revealing a collective character differently from what is observed in Ca$_2$RuO$_4$. Theoretical modelling supports the interpretation of this lowest energy excitation in Ca$_3$Ru$_2$O$_7$ as a magnetic transverse mode with multi-particle character, whereas the corresponding excitation in Ca$_2$RuO$_4$ is assigned to combined longitudinal and transverse spin modes. These fundamental differences are discussed in terms of the inequivalent magnetic ground-state manifestations in Ca$_2$RuO$_4$ and Ca$_3$Ru$_2$O$_7$.
Resonant x-ray diffraction performed at the $rm L_{II}$ and $rm L_{III}$ absorption edges of Ru has been used to investigate the magnetic and orbital ordering in Ca$_2$RuO$_4$ single crystals. A large resonant enhancement due to electric dipole $2pto 4d$ transitions is observed at the wave-vector characteristic of antiferromagnetic ordering. Besides the previously known antiferromagnetic phase transition at $rm T_{N}=110$ K, an additional phase transition, between two paramagnetic phases, is observed around 260 K. Based on the polarization and azimuthal angle dependence of the diffraction signal, this transition can be attributed to orbital ordering of the Ru $t_{2g}$ electrons. The propagation vector of the orbital order is inconsistent with some theoretical predictions for the orbital state of Ca$_2$RuO$_4$.
Low-energy electron excitation spectra were measured on a single crystal of a typical iron-based superconductor PrFeAsO$_{0.7}$ using resonant inelastic X-ray scattering (RIXS) at the Fe-$L_3$ edge. Characteristic RIXS features are clearly observed around 0.5, 1-1.5 and 2-3 eV energy losses. These excitations are analyzed microscopically with theoretical calculations using a 22-orbital model derived from first-principles electronic structure calculation. Based on the agreement with the experiment, the RIXS features are assigned to Fe-$d$ orbital excitations which, at low energies, are accompanied by spin flipping and dominated by Fe $d_{yz}$ and $d_{xz}$ orbital characters. Furthermore, our calculations suggest dispersive momentum dependence of the RIXS excitations below 0.5 eV, and predict remarkable splitting and merging of the lower-energy excitations in momentum space. Those excitations, which were not observed in the present experiment, highlight the potential of RIXS with an improved energy resolution to unravel new details of the electronic structure of the iron-based superconductors.
How coherent quasiparticles emerge by doping quantum antiferromagnets is a key question in correlated electron systems, whose resolution is needed to elucidate the phase diagram of copper oxides. Recent resonant inelastic X-ray scattering (RIXS) experiments in hole-doped cuprates have purported to measure high-energy collective spin excitations that persist well into the overdoped regime and bear a striking resemblance to those found in the parent compound, challenging the perception that spin excitations should weaken with doping and have a diminishing effect on superconductivity. Here we show that RIXS at the Cu L3-edge indeed provides access to the spin dynamical structure factor once one considers the full influence of light polarization. Further we demonstrate that high-energy spin excitations do not correlate with the doping dependence of Tc, while low-energy excitations depend sensitively on doping and show ferromagnetic correlations. This suggests that high-energy spin excitations are marginal to pairing in cuprate superconductors.
By inelastic neutron scattering, we have analyzed the magnetic correlations in the paramagnetic metallic region of the series Ca(2-x)Sr(x)RuO(4), 0.2<=x<=0.62. We find different contributions that correspond to 2D ferromagnetic fluctuations and to fluctuations at incommensurate wave vectors (0.11,0,0), (0.26,0,0) and (0.3,0.3,0). These components constitute the measured response as function of the Sr-concentration x, of the magnetic field and of the temperature. A generic model is applicable to metallic Ca(2-x)Sr(x)RuO(4) close to the Mott transition, in spite of their strongly varying physical properties. The amplitude, characteristic energy and width of the incommensurate components vary only little as function of x, but the ferromagnetic component depends sensitively on concentration, temperature and magnetic field. While ferromagnetic fluctuations are very strong in Ca1.38Sr0.62RuO4 with a low characteristic energy of 0.2 meV at T=1.5 K, they are strongly suppressed in Ca1.8Sr0.2RuO4, but reappear upon the application of a magnetic field and form a magnon mode above the metamagnetic transition. The inelastic neutron scattering results document how the competition between ferromagnetic and incommensurate antiferromagnetic instabilities governs the physics of this system.
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