d-d excitations in manganites probed by resonant inelastic x-ray scattering

We report a study of electronic excitations in manganites exhibiting a range of ground states, using resonant inelastic x-ray scattering (RIXS) at the Mn K edge. Excitations with temperature dependent changes correlated with the magnetism were observed as high as 10 eV. By calculating Wannier functions, and finite-q response functions, we associate this dependence with intersite d-d excitations. The calculated dynamical structure factor is found to be similar to the RIXS spectra.     

Single and double orbital excitations probed by resonant inelastic x-ray scattering

The dispersion of the elusive elementary excitations of orbital ordered systems, orbitons, has escaped detection so far. The recent advances in resonant inelastic x-ray scattering (RIXS) techniques have made it, in principle, a powerful new probe of orbiton dynamics. We compute the detailed traces that orbitons leave in RIXS for an e{g} orbital ordered system, using the ultrashort core-hole lifetime expansion for RIXS. We observe that both single- and double-orbiton excitations are allowed, where the former, at lower energy, have sharper features. The rich energy- and momentum-dependent intensity variations that we observe make clear that RIXS is an ideal method to identify and map out orbiton dispersions.     

Mott gap excitations and resonant inelastic x-ray scattering in doped cuprates

Predictions are made for the momentum- and carrier-dependent degradation of the Mott gap upon doping in high-T(c) 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.     

Low energy electronic excitations in the layered cuprates studied by copper L3 resonant inelastic x-ray scattering

We have measured the resonant inelastic x-ray scattering (RIXS) spectra at the Cu L3 edge in a variety of cuprates. Exploiting a considerably improved energy resolution (0.8 eV) we recorded significant dependencies on the sample composition and orientation, on the scattering geometry, and on the incident photon polarization. The RIXS final states correspond to two families of electronic excitations, having local (dd excitations) and nonlocal (charge-transfer) character. The dd energy splitting can be estimated with a simple crystal field model. The RIXS at the L3 edge demonstrates here a great potential, thanks to the resonance strength and to the large 2p spin-orbit splitting.     

Studies of phononlike low-energy excitations of protein molecules by inelastic x-ray scattering

Molecular dynamics simulations and neutron scattering experiments have shown that many hydrated globular proteins exhibit a universal dynamic transition at TD = 220 K, below which the biological activity of a protein sharply diminishes. We studied the phononlike low-energy excitations of two structurally very different proteins, lysozyme and bovine serum albumin, using inelastic x-ray scattering above and below TD. We found that the excitation energies of the high-Q phonons show a marked softening above TD. This suggests that the large amplitude motions of wavelengths corresponding to this specific Q range are intimately correlated with the increase of biological activities of the proteins.     

Theory of indirect resonant inelastic X-ray scattering

We express the cross section for indirect resonant inelastic X-ray scattering in terms of an intrinsic dynamic correlation function of the system that is studied with this technique. The cross section is a linear combination of the charge response function and the dynamic longitudinal spin density correlation function. This result is asymptotically exact for both strong and weak local core-hole potentials. We show that one can change the relative charge and spin contribution to the inelastic spectral weight by varying the incident photon energy.     

Theory of resonant Raman scattering from low-energy collective excitations of interacting electrons in quantum wires

The Raman spectra of quantum wires in the region of electronic intra-band excitations are investigated using one- and two-band models based on the Luttinger approximation with spin. Structures related to charge and spin density modes are identified, and analyzed with respect to their behavior with photon energy and temperature. It is found that the low-energy peaks in the polarized spectra, close to resonance that are commonly assigned to “single particle excitations”, can be interpreted as the signature of spin density excitations. A broad structure in the resonant depolarized spectrum is predicted above the frequency of the spin density excitations. This is due to simultaneous but independent propagation of spin and charge density modes. The results, when compared with experiment, show, that the electronic collective excitations of quantum wires at low energies are characteristic for a non-Fermi liquid. Received: 25 March 1998 / Accepted: 3 June 1998     

Restoration of selection rules in nonadiabatic resonant inelastic x-ray scattering

Recently a new effect in the Raman scattering of x-ray radiation has been predicted theoretically and discovered in experiments, the effect of restoration of the selection rules for the scattering tensor under strong electron-vibrational interaction. We propose a fairly simple model for describing this effect, a model that allows for an exact solution and takes into account the real vibrational structure of the molecule and electron-vibrational interaction. Zh. éksp. Teor. Fiz. 112, 37–49 (July 1997)     

Linear dichroism in resonant inelastic x-ray scattering to molecular spin-orbit states

Polarization-dependent resonant inelastic x-ray scattering (RIXS) is shown to be a new probe of molecular-field effects on the electronic structure of isolated molecules. A combined experimental and theoretical analysis explains the linear dichroism observed in Cl 2p RIXS following Cl 1s excitation in HCl and CF3Cl as due to molecular-field effects, including singlet-triplet exchange, indicating polarized-RIXS provides a direct probe of spin-orbit-state populations applicable to any molecule.     

Interband collective electronic excitations in resonant Raman scattering of two-subband quantum wires

Using the bosonization technique, a theory for the collective excitations of the interacting electrons in quantum wires with two subbands occupied is developed. The dispersion relations for the inter-subband charge and spin density excitations are determined. The results are used to interpret the features observed in recent measurements of the Raman spectra of AlGaAs/GaAs quantum wires, particularly for photon energies near band gap resonance. It is shown that peaks previously identified as “single particle excitations” are signatures of higher order collective spin density excitations. Predictions about the observability of the interband modes are made. Received 8 February 1999     

Some notes on data analysis for nuclear resonant inelastic x-ray scattering

Nuclear Resonant Inelastic X-ray Scattering (NRIXS) is a spectroscopy method to study atomic vibrations and dynamics, currently done with synchrotron radiation at a few high energy third generation facilities. It finds a wide range of applications in condensed matter physics, materials science, chemistry, biophysics, geosciences, and high-pressure researches. Many atomic dynamics and lattice thermodynamics information can be derived from NRIXS measurements. Phonon Density of States (DOS) characterizes lattice dynamics of a material and can be derived under the quasi-harmonic approximation. Combined with modeling and simulations, results from NRIXS can provide unique and clarifying insights into many fields of research. As for a spectroscopic technique, in order to be able to provide reliable information, close attention should be paid to many issues during experiments and data analysis afterwards. Here we discuss several issues relevant to its data analysis, namely, those of multiple sites, background treatments, and error estimates for some derived quantities.     

Collapse of the magnetic gap of cuprate superconductors within a three-band model of resonant inelastic x-ray scattering

We present a three-band Hubbard Hamiltonian and the associated Cu Kappa-edge resonant inelastic x-ray scattering (RIXS) spectra for electron- and hole-doped cuprates over a wide range of energy and momentum transfers. By comparing computed spectra for the unfilled case with the corresponding results for 15% electron or hole doping at two different values of the effective Hubbard parameter , generic signatures of the collapse of the magnetic gap and the characteristic momentum dependencies and evolution of the spectra with doping are identified. Available RIXS data support the gap collapse scenario for electron-doped cuprates, but the situation in hole-doped systems is found to be less clear.     

Theory of inelastic scattering from magnetic impurities

We use the numerical renormalization group method to calculate the single-particle matrix elements T of the many-body T matrix of the conduction electrons scattered by a magnetic impurity at T=0 temperature. Since T determines both the total and the elastic, spin-diagonal scattering cross sections, we are able to compute the full energy, spin, and magnetic field dependence of the inelastic scattering cross section sigma(inel)(omega). We find an almost linear frequency dependence of sigma(inel)(omega) below the Kondo temperature T(K), which crosses over to a omega(2) behavior only at extremely low energies. Our method can be generalized to other quantum impurity models.     

Angular dependence of resonant inelastic x-ray scattering: a spherical tensor expansion

A spherical tensor expansion is carried out to express the resonant inelastic scattering cross-section as a sum of products of fundamental spectra with tensors involving wavevectors and polarization vectors of incident and scattered photons. The expression presented in this paper differs from that of the influential article by Carra et al. (Phys. Rev. Lett. 74, 3700, 1995) because it does not omit interference terms between electric dipole and quadrupole contributions when coupling each photon to itself. Some specific cases of the spherical tensor expansion are discussed. For example the case of isotropic samples is considered and the cross-section is expressed as a combination of only three fundamental spectra for the situation where electric dipole or electric quadrupole transitions in the absorption process are followed by electric dipole transitions in the emission. This situation includes the case of untextured powder samples, which corresponds to the most frequent situation met experimentally. Finally, it is predicted that some circular dichroism may be observed on isotropic samples provided that the circular polarization of the scattered beam can be detected.     

Momentum dependence of charge excitations in the electron-doped superconductor Nd1.85 Ce0.15 CuO4: a resonant inelastic x-ray scattering study

We report a resonant inelastic x-ray scattering (RIXS) study of charge excitations in the electron-doped high-T(c) superconductor Nd1.85 Ce0.15 CuO4. The intraband and interband excitations across the Fermi energy are separated for the first time by tuning the experimental conditions properly to measure charge excitations at low energy. A dispersion relation with q-dependent width emerges clearly in the intraband excitation, while the intensity of the interband excitation is concentrated around 2 eV near the zone center. The experimental results are consistent with theoretical calculation of the RIXS spectra based on the Hubbard model.