Resonant channel coupling in electron scattering by pyrazine

Detailed investigation of the three low-energy resonances seen in electron scattering by the diazabenzene molecule pyrazine reveals that the first two are nearly pure single-channel shape resonances, but the third is, as long suspected, heavily mixed with core-excited resonances built on low-lying triplet states. Such resonant channel coupling is likely to be widespread in pi-ring molecules, including the nucleobases of DNA and RNA, where it may form a pathway for radiation damage.     

Resonant X-ray magnetic scattering has gone soft

The Linac Coherent Light Source [1] (LCLS) at SLAC National Accelerator Laboratory is preparing for the arrival of its first scientific users in the fall of 2009. LCLS is the world's first free-electron in the spectral range 800?8,000?eV, producing intense, sub-picosecond pulses of Xrays with very high spatial coherence. The accelerator facility has been commissioned in stages, beginning in April 2007 [2] with the injector linac and culminating in December 2008 [3] with the first transport of electrons through the complete beam path. On April 10, 2009, the LCLS Project team was rewarded for years of planning, design, construction, and checkout with a dream-come-true: as undulators were placed on the beam path one-by-one, the laser simply turned on without drama in the course of one hour [4]. First visible evidence of light amplification at 8,000?eV was observed on a fluorescent screen with ten undulators in place, at which point a highly collimated spot of X-rays could be discerned in the center of the spontaneous radiation pattern. After just four days of further checkout, the intensity of this spot increased smoothly and exponentially to the threshold of “saturation” at full power with just 20 of 33 undulators in place. The commissioning team was faced with a mixture of shock and euphoria. The Project team has spent years focused on everything that could possibly go wrong, and what to do about each concern. Speaking for myself, I found I was mentally unprepared for the special case of NOTHING going wrong! In fact, a critical aspect of the FEL performance was significantly better than design goals—the gain length (the distance the electron beam must travel in undulators to increase X-ray power by a factor e) proved to be just 3.5 meters. With this gain length, and room for 33 undulators in the tunnel, we find we have ten more spares! The shutter was closed at about midnight, temporarily preventing the electron beam entering the undulator. At 8:00 A.M. the next morning, the shutter was retracted to reveal the FEL producing an 8,000?eV laser beam without need for operator intervention.     

Resonant elastic X-ray scattering in chemistry and materials science

The applications of anomalous scattering for locating metal atoms and discriminating between different elements has increased when optimised with synchrotron X-radiation.The on-resonance effect enhances the targeted elemental signal and allows small occupancies to be determined, including in situations of a mixed metal population at a single atomic site. Thus the applications of resonant elastic X-ray scattering in biological, inorganic and materials chemistry is being widely applied to single crystals, which is our emphasis, but also powders, fibres, solutions, amorphous and thin film states of matter. Recent developments have included the use of high photon energies (upto 100 keV) as well as softer X-rays (2 keV). The various instrument and technical capabilities have improved in the last 15 years. This ease of measurement of the resonant scattering signals along with absorption edge shifts indicates an expansion to the measurement of multiple data sets, to allow monitoring of redox changes. Whilst crystal structure determination in biological crystallography has been revolutionised by the MAD method, it is not a requirement for chemical or materials crystallography, as other phasing techniques are routine. Synchrotron source upgrades will allow nano-sized X-ray beams to be more widely available. The new X-ray lasers suggest new capabilities too.     

Resonant inelastic X-ray scattering of tantalum double perovskite structures

In this paper, we investigated the electronic structures and defect states of SrLaMgTaO₆ (SLMTO) double perovskite structures by using resonant inelastic x-ray scattering. Recently, Eu³⁺ doped SLMTO red phosphors have been vigorously investigated due to their higher red emission efficiency compared to commercial white light emitting diodes (W-LED). However, a comprehensive understanding on the electronic structures and defect states of host SLMTO compounds, which are specifically related to the W-LED and photoluminescence (PL), is far from complete. Here, we found that the PL spectra of SLMTO powder compounds sintered at a higher temperature, 1400 °C, were weaker in the blue emission regions (at around 400 nm) and became enhanced in near infrared (NIR) regions compared to those sintered at 1200 °C. To elucidate the difference of the PL spectra, we performed resonant inelastic x-ray spectroscopy (RIXS) at Ta L-edge. Our RIXS result implies that the microscopic origin of different PL spectra is not relevant to the Ta-related defects and oxygen vacancies.     

Resonant inelastic X-ray scattering and its magnetic circular dichroism

Magnetic circular dichroism in resonant inelastic X-ray scattering (MCD-RIXS) of ferromagnetic systems is discussed for the longitudinal geometry (LG), where the directions of incident X-ray and magnetization are parallel, and the transverse geometry (TG), where they are perpendicular. MCD-RIXS in LG is represented by two successive real processes, X-ray absorption and X-ray emission, while MCD-RIXS in TG is given by the interference process. We describe an application of MCD-RIXS in LG to the detection of Ce 4f² contribution in Ce, L₃ absorption edge of CeFe₂, and theoretical and experimental studies of MCD-RIXS in TG for Gd and Sm systems.     

Resonant inelastic X-ray scattering of the holon-antiholon continuum in SrCuO2

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, the onset of which exhibits a small dispersion of approximately 0.4 eV. Within this continuum, a highly dispersive feature with a large sinusoidal dispersion (approximately 1.1 eV) is observed. 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 comprises a holon-antiholon continuum together with a broad resonance.     

Resonant scattering of an X-ray photon by a heavy atom

The influence of many-body and relativistic effects on the absolute values and shape of the double differential cross section for the resonant scattering of a linearly polarized X-ray photon by a free xenon atom near the K-shell ionization threshold has been theoretically analyzed. The evolution of the spatially extended structure of the scattering cross section to the K _{α, β} structure of the X-ray spectrum of the xenon atom emission has been demonstrated. The calculations have been performed in the dipole approximation for the anomalous dispersion component of the total inelastic scattering amplitude and in the impulse approximation for the contact component of this amplitude. The contribution of the Rayleigh (elastic) scattering component is taken into account using the methods developed in Hopersky et al., J. Phys. B 30, 5131 (1997). The effects of the radial relaxation of the electron shells, spin-orbit splitting, double excitation/ionization of the atomic ground state, as well as the Auger and radiative decays of the produced main vacancies, are considered. Using the results obtained by Tulkki, Phys. Rev. A 32, 3153 (1985) and Biggs et al., At. Data Nucl. Data Tables 16, 201 (1975), the nonrelativistic Hartree-Fock wavefunctions are changed to the relativistic Dirac-Hartree-Fock wavefunctions of the single-particle scattering states when constructing the process probability amplitude. The calculations are predicting and are in good agreement with the synchrotron experiment on the measurement of the absolute values and shape of the double differential cross section for the resonant scattering of an X-ray photon by a free xenon atom reported by Czerwinski et al., Z. Phys. A 322, 183 (1985).     

Resonant scattering of X-ray radiation in magnetic crystals with non-cubic local anisotropy

Features of resonant diffraction of synchrotron radiation in magnetic crystals in which the local symmetry of resonant atom positions is lower than cubic are considered. It was shown that the simultaneous presence of two anisotropic factors can cause asymmetry of the azimuthal dependence of purely resonant reflections. The observed azimuthal dependence of the 002 reflection in the HoFe₂ crystal was numerically simulated.     

Resonant soft X-ray scattering studies of multiferroic YMn2O5

We performed soft X-ray resonant scattering at the MnL _2,3- and OK edges of YMn₂O₅. While the resonant intensity at the Mn L _2,3 edges reflects the magnetic order parameter, the resonant scattering at the O K edge is found to be directly related to the macroscopic ferroelectric polarization. The latter observation reveals the important role of the spin-dependent Mn-O hybridization for the multiferroicity of YMn₂O₅. We present details about how to obtain correct energy dependent lineshapes and discuss the origin of the resonant intensity at the O K edge.     

Resonant inelastic contact scattering of X-ray photons on atoms and ions

The existence of an extended resonance structure outside the X-ray emission regions is theoretically predicted in the total double differential cross section for the scattering of linearly polarized photons on free atoms (ions). This structure is almost entirely determined by inelastic photon scattering of the contact type. The amplitude of the inelastic contact scattering probability is described using an analytical expression for a non-relativistic transition operator, which was previously obtained by the author outside the dipole and momentum approximations. The resonant inelastic contact scattering of X-ray photons on a neon atom and neonlike ions of argon, titanium, and iron has been studied. Calculations were performed in a nonrelativistic approximation for the wave functions of the scattering states, with allowance for many-body effects of the radial relaxation of one-electron orbitals in the Hartree-Fock field of a deep 1s vacancy and (for neon atom) the double excitation/ionization of the ground atomic state.     

Resonant inelastic scattering of an X-ray photon by a linear molecule

The double differential cross section of resonant inelastic scattering of a linearly polarized X-ray photon by a spatially oriented HF molecule in a gas phase is theoretically described in the energy range of the ionization threshold of the deep molecular orbital 1σ. The effects of radial relaxation of the wave functions of the core and excited scattering states in fields of the formed core vacancies, the vibronic effects, and the effects of Auger and radiative decays of the vacancies are taken into account in the nonrelativistic Hartree-Fock approximation. The results of the calculations are predictive and agree well with the results of the experimental measurements of the Kα emission spectrum of the HF molecule at an incident photon energy of 2 keV, which considerably exceeds the energy of the 1σ ionization threshold.     

Resonant inelastic scattering in dilute magnetic semiconductors by soft X-ray fluorescence spectroscopy

1-x Mn_xS (where 0.05<x<1) were measured as the energy of the exciting radiation was tuned across the S and Mn-L_2,3 absorption edges of these compounds. Strong resonance peaks in Mn-L emission spectra and the systematic appearance of new spectral features in S-L emission spectra were observed. Partial substitution of Zn by a magnetic Mn ion results in strong hybridization of the Mn 3d orbitals with the sp band of the host semiconductor. A detailed study of resonant inelastic scattering in the vicinity of the S and Mn-L_2,3 absorption edges of these DMS is presented. Received: 6 March 1997     

Direct observation of antiferroquadrupolar ordering: resonant X-Ray scattering study of DyB2C2

Antiferroquadrupolar (AFQ) ordering has been conjectured in several rare-earth compounds to explain their anomalous magnetic properties. No direct evidence for AFQ ordering, however, has been reported. Using the resonant x-ray scattering technique near the Dy L(III) absorption edge, we have succeeded in observing the AFQ order parameter in DyB2C2 and analyzing the energy and polarization dependence. The much weaker coupling between the orbital degrees of freedom and the lattice in 4f electron systems than in 3d compounds makes them an ideal platform to study orbital interactions originating from electronic mechanisms.     

Resonant enhancements at nonmagnetic ions: new possibilities for magnetic X-ray scattering

Synchrotron experiments with uranium antiferromagnetic compounds have discovered large ( >1000) enhancements of the magnetic scattering intensities at the K edges of nominally nonmagnetic anions, e.g., Ga and As. The width in energy, the position with respect to the white line, and the azimuthal and polarization dependencies permit one to associate the signal with transitions of E1 dipole symmetry from 1s to 4p states. In momentum space, the signal exhibits long-range order at the antiferromagnetic wave vector. We discuss possible channels capable of generating the observed enhancements.     

Resonant X-ray scattering from a rotating medium: The Nuclear Lighthouse Effect

A coherently excited nuclear state is carried with a rotating sample so that its radiative decay is redirected by the rotation angle that has developed during its lifetime. As a result, the time spectrum of the nuclear decay is mapped to an angular scale. This effect has been observed in nuclear resonant scattering of synchrotron radiation from a rotating ⁵⁷Fe metal foil. Applications with respect to elastic and inelastic nuclear resonant scattering are discussed. This revised version was published online in August 2006 with corrections to the Cover Date.     

Resonant scattering of solitons

We study the scattering of solitons in the nonlinear Schr?dinger equation on local inhomogeneities which may give rise to resonant transmission and reflection. In both cases, we derive resonance conditions for the soliton's velocity. The analytical predictions are tested numerically in regimes characterized by various time scales. Special attention is paid to intermode interactions and their effect on coherence, decoherence, and dephasing of plane-wave modes which build up the soliton.