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D. Casa

Publications and source records attributed to D. Casa.

At least 37 records · Page 2Linked to original sources

Resonant inelastic x-ray scattering study of electronic excitations in insulating K$_{0.83}$Fe$_{1.53}$Se$_2$

We report an Fe $K$-edge resonant inelastic X-ray scattering (RIXS) study of K$_{0.83}$Fe$_{1.53}$Se$_2$. This material is an insulator, unlike many parent compounds of iron-based superconductors. We found a sharp excitation around 1 eV, which is resonantly enhanced when the incident photon energy is tuned near the pre-edge region of the absorption spectrum. The spectral weight and line shape of this excitation exhibit clear momentum dependence. In addition, we observe momentum-independent broad interband transitions at higher excitation energy of 3-7 eV. Calculations based on a 70 band $dp$ orbital model, using a moderate $U_{\rm eff}\approx 2.5$ eV, indicate that the $\sim$1 eV feature originates from the correlated Fe 3$d$ electrons, with a dominant $d_{xz}$ and $d_{yz}$ orbital character. We find that a moderate $U_{\rm eff}$ yields a satisfying agreement with the experimental spectra, suggesting that the electron correlations in the insulating and metallic iron based superconductors are comparable.

cond-mat.supr-con↗

Tuning Magnetic Coupling in Sr$_2$IrO$_4$ Thin Films with Epitaxial Strain

We report x-ray resonant magnetic scattering (XRMS) and resonant inelastic x-ray scattering (RIXS) studies of epitaxially-strained $\mathrm{Sr_2IrO_4}$ thin films. The films were grown on $\mathrm{SrTiO_3}$ and $\mathrm{(LaAlO_3)_{0.3}(Sr_2AlTaO_6)_{0.7}}$ substrates, under slight tensile and compressive strains, respectively. Although the films develop a magnetic structure reminiscent of bulk $\mathrm{Sr_2IrO_4}$, the magnetic correlations are extremely anisotropic, with in-plane correlation lengths significantly longer than the out-of-plane correlation lengths. In addition, the compressive (tensile) strain serves to suppress (enhance) the magnetic ordering temperature $\mathrm{T_N}$, while raising (lowering) the energy of the zone boundary magnon. Quantum chemical calculations show that the tuning of magnetic energy scales can be understood in terms of strain-induced change in bond lengths.

cond-mat.str-el↗

Dilute Magnetism and Spin-Orbital Percolation Effects in Rh-doped Sr2IrO4

We have used a combination of resonant magnetic x-ray scattering (RMXS) and x-ray absorption spectroscopy (XAS) to investigate the properties of the doped spin-orbital Mott insulator Sr2Ir(1-x)Rh(x)O4 (0.07 < x < 0.70). We show that Sr2Ir(1-x)Rh(x)O4 represents a unique model system for the study of dilute magnetism in the presence of strong spin-orbit coupling, and provide evidence of a doping-induced change in magnetic structure and a suppression of magnetic order at x_c ~ 0.17. We demonstrate that Rh-doping introduces Rh3+/Ir5+ ions which effectively hole-dope this material. We propose that the magnetic phase diagram for this material can be understood in terms of a novel spin-orbital percolation picture.

cond-mat.str-el↗

Ferromagnetic Exchange Anisotropy from Antiferromagnetic Superexchange in the Mixed 3d-5d Transition-Metal Compound Sr3CuIrO6

We report a combined experimental and theoretical study of the unusual ferromagnetism in the one-dimensional copper-iridium oxide Sr$_3$CuIrO$_6$. Utilizing Ir $L_3$ edge resonant inelastic x-ray scattering, we reveal a large gap magnetic excitation spectrum. We find that it is caused by an unusual exchange anisotropy generating mechanism, namely, strong ferromagnetic anisotropy arising from antiferromagnetic superexchange, driven by the alternating strong and weak spin-orbit coupling on the $5d$ Ir and 3d Cu magnetic ions, respectively. From symmetry consideration, this novel mechanism is generally present in systems with edge-sharing Cu$^{2+}$O$_4$ plaquettes and Ir$^{4+}$O$_6$ octahedra. Our results point to unusual magnetic behavior to be expected in mixed 3d-5d transition-metal compounds via exchange pathways that are absent in pure 3d or 5d compounds.

cond-mat.str-el↗

Magnetic excitation spectrum of Na2IrO3 probed with resonant inelastic x-ray scattering

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 strong electron-lattice coupling is present in Na2IrO3.

cond-mat.str-el↗

Resonant inelastic X-ray scattering study of intra-band charge excitations in hole-doped high-Tc cuprates

We have performed resonant inelastic x-ray scattering (RIXS) near the Cu-K edge on cuprate superconductors La(2-x)Sr(x)CuO(4), La(2-x)Ba(x)CuO(4), La(2-x)Sr(x)Cu(1-y)Fe(y)O(4) and Bi(1.76)Pb(0.35)Sr(1.89)CuO(6+d), covering underdoped to heavily overdoped regime and focusing on charge excitations inside the charge-transfer gap. RIXS measurements of the 214 systems with Ei = 8.993 keV have revealed that the RIXS intensity at 1 eV energy transfer has a minimum at (0,0) and maxima at (0.4pi, 0) and $(0, 0.4pi) for all doping points regardless of the stripe ordered state, suggesting that the corresponding structure is not directly related to stripe order. Measurements with Ei = 9.003 keV on metallic La(1.7)Sr(0.3)CuO(4) and Bi(1.76)Pb(0.35)Sr(1.89)CuO(6+d) exhibit a dispersive intra-band excitation below 4 eV, similar to that observed in the electron-doped Nd(1.85)Ce(0.15)CuO(4). This is the first observation of a dispersive intra-band excitation in a hole doped system, evidencing that both electron and hole doped systems have a similar dynamical charge correlation function.

cond-mat.supr-con↗

Spin-state transition in the Fe-pnictides

We report a Fe Kβx-ray emission spectroscopy study of local magnetic moments in the rare-earth doped iron pnictide Ca_{1-x}RE_xFe_2As_2 (RE=La, Pr, and Nd). In all samples studied the size of the Fe local moment is found to decrease significantly with temperature and goes from ~0.9 μ_B at T = 300 K to ~0.45 μ_B at T = 70 K. In the collapsed tetragonal (cT) phase of Nd- and Pr-doped samples (T<70K) the local moment is quenched, while the moment remains unchanged for the La-doped sample, which does not show lattice collapse. Our results show that Ca_{1-x}RE_xFe_2As_2 (RE= Pr and Nd) exhibits a spin-state transition and provide direct evidence for a non-magnetic Fe^{2+} ion in the cT-phase, as predicted by Yildirim. We argue that the gradual change of the the spin-state over a wide temperature range reveals the importance of multiorbital physics, in particular the competition between the crystal field split Fe 3d orbitals and the Hund's rule coupling.

cond-mat.supr-con↗

Strongly momentum-dependent screening dynamics in La$_{0.5}$Sr$_{1.5}$MnO$_4$ observed with resonant inelastic x-ray scattering

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.

cond-mat.str-el↗

Testing the validity of the strong spin-orbit-coupling limit for octahedrally coordinated iridates in a model system Sr$_3$CuIrO$_6$

The electronic structure of Sr$_3$CuIrO$_6$, a model system for the 5d Ir ion in an octahedral environment, is studied through a combination of resonant inelastic x-ray scattering (RIXS) and theoretical calculations. RIXS spectra at the Ir L$_3$-edge reveal an Ir $t_{2g}$ manifold that is split into three levels, in contrast to the expectations of the strong spin-orbit-coupling limit. Effective Hamiltonian and $ab inito$ quantum chemistry calculations find a strikingly large non-cubic crystal field splitting comparable to the spin-orbit coupling, which results in a strong mixing of the $j_{\mathsf{eff}}=1/2$ and $j_{\mathsf{eff}}=3/2$ states and modifies the isotropic wavefunctions on which many theoretical models are based.

cond-mat.str-el↗

Crystal field splitting and correlation effect on the electronic structure of A2IrO3

The electronic structure of the honeycomb lattice iridates Na2IrO3 and Li2IrO3 has been investigated using resonant inelastic x-ray scattering (RIXS). Crystal-field split d-d excitations are resolved in the high-resolution RIXS spectra. In particular, the splitting due to non-cubic crystal fields, derived from the splitting of j_eff=3/2 states, is much smaller than the typical spin-orbit energy scale in iridates, validating the applicability of j_eff physics in A2IrO3. We also find excitonic enhancement of the particle-hole excitation gap around 0.4 eV, indicating that the nearest-neighbor Coulomb interaction could be large. These findings suggest that both Na2IrO3 and Li2IrO3 can be described as spin-orbit Mott insulators, similar to the square lattice iridate Sr2IrO4.

cond-mat.str-el↗

Giant Magnon Gap in Bilayer Iridate Sr3Ir2O7: Enhanced Pseudo-dipolar Interactions Near the Mott Transition

Using resonant inelastic x-ray scattering, we observe in the bilayer iridate Sr3Ir2O7, a spin-orbit coupling driven magnetic insulator with a small charge gap, a magnon gap of ~92 meV for both acoustic and optical branches. This exceptionally large magnon gap exceeds the total magnon bandwidth of ~70 meV and implies a marked departure from the Heisenberg model, in stark contrast to the case of the single-layer iridate Sr2IrO4. Analyzing the origin of these observations, we find that the giant magnon gap results from bond-directional pseudo-dipolar interactions that are strongly enhanced near the metal-insulator transition boundary. This suggests that novel magnetism, such as that inspired by the Kitaev model built on the pseudo-dipolar interactions, may emerge in small charge-gap iridates.

cond-mat.str-el↗

Isospin Dynamics in Sr2IrO4 : Forging Links to Cuprate Superconductivity

We used resonant inelastic x-ray scattering to reveal the nature of magnetic interactions in Sr2IrO4, a 5d transition-metal oxide with a spin-orbit entangled ground state and Jeff=1/2 magnetic momemts, referred to as 'isospins'. The magnon dispersion in Sr2IrO4 is well described by an antiferromagnetic Heisenberg model with isospin one-half moments on a square lattice, which renders the low-energy effective physics of Sr2IrO4 much akin to that in superconducting cuprates. This is further supported by the observation of exciton modes in Sr2IrO4 whose dispersion is strongly renormalized by magnons, which can be understood by analogy to the hole propagation in the background of antiferromagnetically ordered spins in the cuprates.

cond-mat.str-el↗

Revealing the dual nature of magnetism in iron pnictides and iron chalcogenides using x-ray emission spectroscopy

We report Fe K beta x-ray emission spectroscopy study of local magnetic moments in various iron based superconductors in their paramagnetic phases. Local magnetic moments are found in all samples studied: PrFeAsO, Ba(Fe,Co)2As2, LiFeAs, Fe1+x(Te,Se), and A2Fe4Se5 (A=K, Rb, and Cs). The moment size varies significantly across different families. Specifically, all iron pnictides samples have local moments of about 1 $μ_B$/Fe, while FeTe and K2Fe4Se5 families have much larger local moments of ~2$μ_B$/Fe, ~3.3$μ_B$/Fe, respectively. In addition, we find that neither carrier doping nor temperature change affects the local moment size.

cond-mat.supr-con↗

X-ray induced electronic structure change in CuIr$_2$S$_4$

The electronic structure of CuIr$_2$S$_4$ has been investigated using various bulk-sensitive x-ray spectroscopic methods near the Ir $L_3$-edge: resonant inelastic x-ray scattering (RIXS), x-ray absorption spectroscopy in the partial fluorescence yield (PFY-XAS) mode, and resonant x-ray emission spectroscopy (RXES). A strong RIXS signal (0.75 eV) resulting from a charge-density-wave gap opening is observed below the metal-insulator transition temperature of 230 K. The resultant modification of electronic structure is consistent with the density functional theory prediction. In the spin- and charge- dimer disordered phase induced by x-ray irradiation below 50 K, we find that a broad peak around 0.4 eV appears in the RIXS spectrum.

cond-mat.str-el↗

Electronic Structure of Doped Lanthanum Cuprates Studied with Resonant Inelastic X-Ray Scattering

We report a comprehensive Cu $K$-edge RIXS investigation of $\rm La_{2-x}Sr_xCuO_4$ (LSCO) for 0$\leq$x$\leq$0.35, stripe-ordered $\rm La_{1.875}Ba_{0.125}CuO_4$ (LBCO), and $\rm La_{2}Cu_{0.96}Ni_{0.04}O_4$ (LCNO) crystals. The RIXS spectra measured at three high-symmetry momentum transfer (\textbf{q}) positions are compared as a function of doping and for the different dopants. The spectra in the energy range 1-6 eV can be described with three broad peaks, which evolve systematically with increased doping. The most systematic trend was observed for \textbf{q}=($π$, 0) corresponding to the zone boundary. As hole doping increased, the spectral weight transfer from high energies to low energies is nearly linear with \emph{x} at this \textbf{q}. We interpret the peaks as interband transitions in the context of existing band models for this system, assigning them to Zhang-Rice band$\rightarrow$upper Hubbard band, lower-lying band$\rightarrow$upper Hubbard band, and lower-lying band$\rightarrow$Zhang-Rice band transitions. The spectrum of stripe-ordered LBCO was also measured, and found to be identical to the correspondingly doped LSCO, except for a relative enhancement of the near-infrared peak intensity around 1.5-1.7 eV. The temperature dependence of this near-infrared peak in LBCO was more pronounced than for other parts of the spectrum, continuously decreasing in intensity as the temperature was raised from 25 K to 300 K. Finally, we find that 4\% Ni substitution in the Cu site has a similar effect on the spectra as does Sr substitution in the La site.

cond-mat.str-el↗

d-d Excitations in Bilayer Manganites Probed by Resonant Inelastic X-ray Scattering

We report a high resolution resonant inelastic x-ray scattering investigation of the bilayer manganites La$_{2-2x}$Sr$_{1+2x}$Mn$_2$O$_7$ with $x = 0.36$ and $0.5$. The momentum dependence along the crystallographic $(110)$ direction for energy losses $1\,\rm{eV} \leq ΔE \leq 15\,\rm{eV}$ has been measured in detail with the data analysis focusing on the energy loss region $1\,\rm{eV} \leq ΔE \leq 5\,\rm{eV}$, which includes a strong peak located at $ΔE \approx 2\,\rm{eV}$. We observe a clear dispersion of up to $0.5\,\rm{eV}$ in the measured $\textbf{q}$ range, which is direct evidence of the non-local character of this excitation. Further, we found that the intensity in this low energy region strongly depends on both the reduced wave vector $\textbf{q} = (h, h, 0)$, $h = 0.1 - 0.5$, and temperature, i.e. different ordered phases. Results can be explained via an intersite $d-d$ charge transfer excitation, proposed for pseudo-cubic manganites, where the hopping rate is strongly increased (decreased) by ferromagnetic (antiferromagnetic) alignment of neighboring in-plane Mn ion core spins.

cond-mat.str-el↗

Magnetic nature of the 500 meV peak in $\rm La_{2-x}Sr_{x}CuO_4$ observed with resonant inelastic x-ray scattering at the Cu $K$-edge

We present a comprehensive study of the temperature and doping dependence of the 500 meV peak observed at ${\bf q}=(π,0)$ in resonant inelastic x-ray scattering (RIXS) experiments on $\rm La_2CuO_4$. The intensity of this peak persists above the Néel temperature (T$_{N}$=320 K), but decreases gradually with increasing temperature, reaching zero at around T=500 K. The peak energy decreases with temperature in close quantitative accord with the behavior of the two-magnon $\rm B_{1g}$ Raman peak in $\rm La_2CuO_4$, and with suitable rescaling, agrees with the Raman peak shifts in $\rm EuBa_2Cu_3O_6$ and $\rm K_2NiF_4$. The overall dispersion of this excitation in the Brillouin zone is found to be in agreement with theoretical calculations for a two-magnon excitation. Upon doping, the peak intensity decreases analogous to the Raman mode intensity and appears to track the doping dependence of the spin correlation length. Taken together, these observations strongly suggest that the 500 meV mode is magnetic in character and is likely a two-magnon excitation.

cond-mat.str-el↗

Ultrafast Imaging and the "Phase Problem" for Inelastic X-Ray Scattering

We describe a new method for imaging ultrafast dynamics in condensed matter using inelastic x-ray scattering (IXS). We use the concepts of causality and irreversibility to construct a general solution to the inverse scattering problem (or "phase problem") for inelastic x-ray scattering, which enables direct imaging of dynamics of the electron density with resolutions of ~1 attosecond (10-18 sec) in time and < 1 A in space. This method is not a Fourier transform of IXS data, but a means to impose causality on the data and reconstruct the charge propagator. The method can also be applied to inelastic electron or neutron scattering. We give a general outline of phenomena that can and cannot be studied with this technique, and provide an outlook for the future.

cond-mat.other↗