Polarization dependence of resonant inelastic X-ray scattering spectroscopy in correlated electron systems

Resonant inelastic X-ray scattering (RIXS) at the transition-metal K-edge is studied as a tool to detect the electronic structure in correlated electron systems. We, in particular, focus on the polarization dependence of RIXS intensity and symmetry of the electronic excitations. It is shown that by analyzing the polarization of the initial and scattered X-rays, the symmetry of the 4p orbitals are selected. Combined effects of the polarization of X-rays and the momentum transfer in the scattering are also studied.     

Electron decay following the N 1s→π* excitation in N2 studied under resonant Raman conditions

We have measured decay spectra following the N 1s→π* transition in N₂ with vibrational resolution in both the intermediate and final states. Using photon energy steps of 60 meV subtle changes in both the participator and spectator lines were observed. In particular, spectra measured at photon energies on the low-energy side of the first vibrational component of the absorption curve (“detuning”) gave rise to vibrational collapse of the participator lines. At higher photon energies vibrational-lifetime interference is observed on both participator and spectator lines.     

On the valence states of cerium in CeO2

The absorption spectra below the 4d threshold of cerium in Ce metal, CeF₃ and CeO₂ compounds were measured by using a CDM (Constant Deviation Monochromator) at the Photon Factory, KEK. The difference in structure between these spectra is discussed. The structure appeared in CeO₂ were considered to be due to the tetravalent configuration of cerium (Ce⁴⁺) in the ground state.     

Electronic excitations in hole-doped La1−xSrxMnO3 studied by resonant inelastic X-ray scattering

We report a resonant inelastic X-ray scattering (RIXS) study on perovskite manganese oxides La_1−xSr_xMnO₃ (x=0, 0.2, and 0.4) at Mn K-absorption edge. Hole-doping effect on the electronic excitations in the strongly correlated electron systems is elucidated by comparing with undoped LaMnO₃. The scattering spectra of metallic La_0.6Sr_0.4MnO₃ 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 spectral weight shifts toward lower energies. Though the peak position of the excitations shows weak dispersion in momentum dependence, RIXS intensity changes as a function of the scattering angle (2θ), which is related to the anisotropy. Furthermore, anisotropic temperature dependence is observed in La_0.8Sr_0.2MnO₃ which shows a metal-insulator transition associated with a ferromagnetic transition. We consider that the anisotropy in the RIXS spectra is possibly attributed to the correlation of the orbital degrees of freedom. The anisotropy is large in LaMnO₃ with long-range orbital order, while it is small but finite in hole-doped La_1−xSr_xMnO₃ which indicates persistence of short-range orbital correlation.     

Resonant inelastic x‐ray scattering from highly correlated dysprosium compounds

Dy₂O₃ and Dy metal's resonant inelastic x‐ray scattering (RIXS) spectra were measured in the Beijing Synchrotron Radiation Facility. As a bulk sensitive probe and two‐photon process, RIXS provides more information on the electronic structure of matter. In this full RIXS experiment, the 2p⁶4fⁿ→ 2p⁵4fⁿ5d¹ (2p⁵4f^{n + 1}5d⁰) → 2p⁶3d⁹4fⁿ5d¹ (2p⁶3d⁹4f^{n + 1}5d⁰) channel of two samples (Dy₂O₃ and Dy metal) was studied. Further comparison shows that there are many differences in the RIXS spectra. Dy metal has only a single resonance and its 5d band is broader than that of Dy₂O₃. In the resonant regime, it has a lower final state energy, whereas in the non‐resonant regime it exceeds Dy₂O₃. This causes a broader bandwidth of the main final state B and a narrower bandwidth in the resonant and non‐resonant regime. The pre‐edge structure in Dy L₃ absorption spectra was also resolved using RIXS, which cannot be seen in conventional XAS owing to 2p core hole lifetime broadening. Copyright © 2005 John Wiley & Sons, Ltd.     

Absorption spectroscopic study of the conduction band of titanium dichalcogenides

The L _{2, 3} spectra of titanium in the layered compound TiSe₂ and intercalated compounds Fe_1/2TiSe₂, Cr_1/3TiSe₂, and Fe_1/4TiTe₂ are studied. Theoretical calculations of the electronic structure of these compounds are performed. The experimental data and calculations suggest that the intercalation of the Cr and Fe atoms into the TiSe₂ matrix brings about a partial filling of the Ti 3d states and the spin polarization of the Cr 3d and Fe 3d states. Chemical bonds are formed through the hybridization of the d orbitals of intercalated atoms with the Ti 3d-Se 4p states of the matrix.     

硫化锰电子结构的软X射线共振非弹性散射研究

利用软X射线共振非弹性散射谱(resonant inelastic soft X-ray scattering, RIXS)对3d过渡金属硫化物中的硫化锰(MnS)电子结构进行了研究.通过分析Mn²⁺的2p⁶3d⁵→2p⁵3d⁶→2p⁶3d⁵二次光子过程，得到了共振非弹性散射谱中的两类非弹性峰，d-d电子跃迁和电荷转移(charge-transfer)跃迁.这两部分跃迁分别共振增强于L边附近及伴随峰附近.基于Hartree-Fock方法的多重态计算分别模拟了原子近似下和立方体O_h对称群下共振非弹性散射谱及吸收谱.计算得MnS实际晶体场10Dq值介于0.80eV—0.85eV之间.对MnS和MnO CT跃迁差异的讨论表明MnS较强的CT跃迁来源于其较窄的能隙宽度. 关键词： 软X射线共振非弹性散射 软X射线吸收谱 d-d跃迁 电荷转移     

Charge-transfer excitations in the model superconductor HgBa(2)CuO(4+delta)

We report a Cu -edge resonant inelastic x-ray scattering (RIXS) study of charge-transfer excitations in the 2-8 eV range in the structurally simple compound HgBa(2)CuO(4+delta) at optimal doping (T(c)=96.5 K). The spectra exhibit a significant dependence on the incident photon energy which we carefully utilize to resolve a multiplet of weakly dispersive (<0.5 eV) electron-hole excitations, including a mode at 2 eV. The observation of this 2 eV excitation suggests the existence of a remnant charge-transfer gap deep in the superconducting phase. Quite generally, our results, which include additional data for the Mott insulator La(2)CuO(4), demonstrate the importance of exploring the incident photon-energy dependence of the RIXS cross section.     

Photoemission studies of single crystals of titanium carbide

The electron distribution in the valence band from single crystals of titanium carbide has been studied by photoelectron spectroscopy with photon energies h?ω = 16.8, 21.2, 40.8 and 1486.6 eV. The most conspicious feature of the electron distribution curves for TiC is a hybridization between the titanium 3d and carbon 2p states at ca. 3–4-eV binding energy, and a single carbon 2s band at ca. 10 eV. By taking into account the strong symmetry and energy dependence of the photoionization crosssections, as well as the surface sensitivity, we have identified strong emission from a carbon 2p band at ? 2.9-eV energy. Our results are compared with several recent energy band structure calculations and other experimental data. Results from pure titanium, which have been used for reference purposes, are also presented.The valence band from single crystals of titanium carbide have been studied by means of photoelectron spectroscopy, with photon energies ranging from 16.8 to 1486.6 eV.By taking into account effects such as the symmetry and energy dependence of the photoionization cross-sections and surface sensitivity, we have found the valence band of titanium carbide to consist of two peaks. The upper part of the valence band at 3–4 eV below the Fermi level consists of a hybridization between Ti 3d and C 2p states. The C 2p states observed in our spectra were mainly excited from a band about 2.9 eV below the Fermi level. The APW^5–9, MAPW¹⁰ and EPM¹¹ band structure calculations predict a flat band of p-character between the symmetry points X′₄ and K₃, most likely responsible for the majority of C 2p excitations observed. The C 2s states, on the other hand, form a single band centered around ?10.4 eV.The results obtained are consistent with several recent energy band structure calculations^{5–11, 13} that predict a combined bonding of covalent, ionic and metallic nature.     

Scandium and lutetium surfaces studied by reflection electron energy-loss spectroscopy

The reflection electron energy-loss spectra of the (1 0 0) and (0 0 1) surfaces of Sc single crystals and the (0 0 1) surface of a Lu single crystal have been studied with primary energies in the range 50–2000 eV. Scandium is congeneric with lutetium and the loss spectra of the two elements are very similar in both the collective excitations and the interband transitions. Strong excitations observed at around 41 eV are attributed to 3p → 3d and 5p → 5d transitions in Sc and Lu, respectively. The loss data of Sc fit the characteristic energy-loss data of the other elements of the first group of transition metals. Oxygen adsorption and nitrogen adsorption on the (1 0 0) surface of Sc influence the loss spectra. The observed differences are correlated with density-of-states calculations for Sc, ScO and ScN.     

A study of final state structure in the x-pe spectra of the rare earth oxides,Part III: Ionisation of a 4d electron

Metal 4d photoelectron spectra of the lanthanoid oxides Ln₂O₃ are reported. The 4d signals are complex, showing subsidiary structure due both to electrostatic interactions within the 4d⁹4?ⁿ configurations and to accompanying O 2p → Ln 4? charge-transfer excitations (shake-up). The effects of electrostatic coupling, including configuration interaction in the final state, are analysed in terms of a simple model.     

The model of the optical switching center and the polarization anomalies in absorption spectra of cupric oxide after fast particles irradiation

We consider the model of the optical switching center—a system with the following properties: it has two (or more) metastable states |1〉, |2〉, separated by a potential barrier U; it can switch from one state to another by absorbing the photons with energy ?ω∼U; the transition |1〉→|2〉 is allowed only for a certain light wave polarization p₁ and the transition |2〉→|1〉—for other polarization p₂; these polarizations p₁, p₂ are orthogonal. The optical properties of this system are studied and are found to exhibit unconventional polarization dependence. In particular, the absorption spectrum observed in natural (unpolarized) light can display new features, that are absent in the spectra, obtained in two independent polarizations. We discuss these results in connection with the (yet unexplained) experimental findings [N.N. Loshkareva, Yu.P. Sukhorukov, B.A. Gizhevskii, A.S. Moskvin, T.A. Belykh, S.V. Naumov, A.A. Samokhvalov, Phys. Solid State 40 (1998) 383], where the similar anomalous polarization dependence of the absorption spectra of cupric monoxide CuO after the fast particle bombardment is reported.     

High-spin levels in137,139Ce and139,141Nd evidence for hole-core coupling

Excited states of the¹³⁷Ce,¹³⁹Ce,¹³⁹Nd and¹⁴¹Nd nuclei have been studied using the¹³⁸Ba(α, 5nγ)¹³⁷Ce,¹³⁸Ba(³He, 4nγ)¹³⁷Ce,¹³⁸Ba(α, 3nγ)¹³⁹Ce,¹⁴⁰Ce(α, 5nγ)¹³⁹Nd,¹⁴⁰Ce(³He,4nγ)¹³⁹Nd,¹⁴⁰Ce(α, 3nγ)¹⁴¹Nd and¹⁴²Ce(α, 5nγ)¹⁴¹Nd reactions. Singlesγ-ray spectra,γ —γ coincidence spectra, angular distributions and time distributions ofγ-rays with respect to beam pulses have been measured. Gamma transitions between excited states with spin values up to 21/2, 23/2 or 25/2 have been observed. Isomeric states with T_1/2=70 ns have been observed in¹³⁹Ce at 2631.5 keV (19/2) and in¹⁴¹Nd probably at 2952.0 keV (19/2). The level structure observed in the nuclei studied can be explained if the neutron-holes are coupled to the doubly even core excitations. The coupling of theh _11/2 neutron-hole with the 2⁺, 4⁺ and 3^? collective excitations are calculated in terms of the weak and intermediate coupling models. The intermediate coupling results seem to be in better agreement with the experimental data. The energies of theree-particle states, being the result of the coupling of theh _11/2 neutron-hole with the two-proton excitations in the core, are well reproduced in the calculations when empirical values of the two-body interaction matrix elements were used.     

Breakdown of the one electron approximation for 4p core electron energy loss spectra in the rare earths

At high incident electron energies the 4p core electron energy loss features of clean La, Ce and Gd strongly resemble the corresponding XPS spectrum with evidence of strong 4p^-1 ? 4d^-2?f giant Coster-Kronig resonance in the “4p_{$\text{1}\text{2}$}” spectrum. The absence of charge transfer screening peaks in the $\text{4p}{}_{\mathrm{<mtext>3</mtext><mtext>2</mtext>}}$ loss of the oxides is attributed to localised 4p → 5d¹ excitation. As the primary energy approaches threshold, a satellite on the low energy side of the $\text{4p}{}_{\mathrm{<mtext>3</mtext><mtext>2</mtext>}}$ losses of La and Ce grows in intensity, due to excitations of multiples through non-dipole transitions.     

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.     

Low energy electronic spectroscopy of an infinite-layer cuprate: A resonant inelastic X-ray scattering study of CaCuO2

We report the results of Oxygen K-edge soft X-ray absorption and emission spectroscopy that was performed on an infinite-layer insulating cuprate thin film CaCuO₂. Experimentally obtained spectra are consistent with local density approximation calculations. X-ray absorption spectra show a close resemblance to spectra obtained from homologous single crystal cuprates. In addition to d–d excitations, X-ray emission spectra reveal the presence of Zhang-Rice singlet states in the infinite-layer CuO₂ planes. The question of whether the Zhang-Rice singlet features are masked by the O 2p main-band is addressed: it is possible to quantify the position of the Zhang-Rice singlet using emission intensity profiles. X-ray emission is demonstrated as a tool for understanding CuO₂ planar electronic correlation in the prototypical infinite-layer. The energy difference, 2.0 eV, between the oxygen main-band and the Zhang-Rice singlet band is found to match values obtained theoretically using established planar electronic correlation parameters.     

Single-particle quadrupole electromagnetic transitions in p-shell and sd-shell nuclei

Electron scattering Coulomb form factors for the single-particle quadrupole transitions in p-shell and sd-shell nuclei have been studied. Core polarization effects are included through a microscopic theory that includes excitations from the core orbits up to higher orbits with 2ω excitations. The modified surface delta interaction is adopted as a residual interaction. The results are discussed for the ( 1p _1/2 ^-1↦1p _3/2 ^-1) proton transition in ¹⁵N, ( 1d _5/2↦2s _1/2) neutron transition in ¹⁷O and ( 1d _3/2 ^-1↦2s _1/2 ^-1) proton transition in ³⁹K. The inclusion of core polarization effects modifies the form factors markedly and describes the experimental data very well in both the absolute strength and the momentum transfer dependence. Received: 18 April 2002 / Accepted: 1 July 2002 / Published online: 6 March 2003 RID="a" ID="a"e-mail: baguniv@uruklink.net Communicated by A. Molinari     

The microwave spectrum of α-d2 oxetane and the analysis of the centrifugal distortion constants of oxetane

The microwave spectrum of the α-d₂ isotopic species of oxetane (trimethylene oxide) has been observed from 26.5 to 40.0 GHz. About 60 lines have been assigned for each of v = 0 to v = 5 in the puckering vibration. The spectra have been interpreted using an effective hamiltonian for each vibrational state including four of the five quartic distortion constants according to Watson's formulation. In general, the lines are fitted to better than ±10 kHz.The zig-zag dependence of the distortion constants on the puckering vibrational quantum number has been quantitatively analyzed for the parent, α-d₂, αα′-d₄, d₆, and α-d₂ species of oxetane and has yielded values for the $\text{a}{}_{\mathrm{<mtext>pucker</mtext>}}{}^{\mathrm{\alpha \beta }}$ constants of these isotopic species.     

Calculation of X-ray and Auger transition rates, lifetimes, X-ray wavelengths, and fluorescence yields of variously ionized silicon atoms

X-ray and Auger transition rates, X-ray wavelengths, and fluorescence yields are calculated for variously ionized silicon atoms with configurations 1s2s^m2pⁿ, m=0-2, n=1-6. The calculation has been performed using the Hartree-Fock atomic model. Intermediate coupling and configuration interaction have been taken into account. The energies and widths are found to be strongly affected by configuration mixing. The results from the present calculation have been compared with those available in the literature. The theoretical K_α hypersatellite and satellite spectra fall into several well-separated regions, corresponding to each of the possible number of spectator electrons in the 2s and 2p shells. The dependence of radiative rates and fluorescence yields on the number of spectator electrons is also investigated.     

Polarization transfer in the deuteron break-up reaction at 56 MeV

The polarization transfer coefficients K^yy′ of the break-up spectra in the reactions ¹²C, ⁵⁸Ni, ²⁰⁹Bi($\text{d}$, $\text{p}$X) were measured at 56 MeV. In the forwardd angles (13.5° and 20.0°), the K_y^y′ data at the break-up peak are nearly equal to $\text{2}\text{3}$ (the spectator model prediction) and they decrease at both sides of the peak. The deviation due to the deuteron D-state is estimated, using PWBA and DWBA.