X-ray Linear Dichroism in cubic compounds: the case of Cr3+ in MgAl2O4

The angular dependence (x-ray linear dichroism) of the Cr K pre-edge in MgAl2O4:Cr3+ spinel is measured by means of x-ray absorption near edge structure spectroscopy (XANES) and compared to calculations based on density functional theory (DFT) and ligand field multiplet theory (LFM). We also present an efficient method, based on symmetry considerations, to compute the dichroism of the cubic crystal starting from the dichroism of a single substitutional site. DFT shows that the electric dipole transitions do not contribute to the features visible in the pre-edge and provides a clear vision of the assignment of the 1s-->3d transitions. However, DFT is unable to reproduce quantitatively the angular dependence of the pre-edge, which is, on the other side, well reproduced by LFM calculations. The most relevant factors determining the dichroism of Cr K pre-edge are identified as the site distortion and 3d-3d electronic repulsion. From this combined DFT, LFM approach is concluded that when the pre-edge features are more intense than 4 % of the edge jump, pure quadrupole transitions cannot explain alone the origin of the pre-edge. Finally, the shape of the dichroic signal is more sensitive than the isotropic spectrum to the trigonal distortion of the substitutional site. This suggests the possibility to obtain quantitative information on site distortion from the x-ray linear dichroism by performing angular dependent measurements on single crystals

Experimental evidence of thermal fluctuations on the X-ray absorption near-edge structure at the aluminum K-edge

After a review of temperature-dependent experimental x-ray absorption near-edge structure (XANES) and related theoretical developments, we present the Al K-edge XANES spectra of corundum and beryl for temperature ranging from 300K to 930K. These experimental results provide a first evidence of the role of thermal fluctuation in XANES at the Al K-edge especially in the pre-edge region. The study is carried out by polarized XANES measurements of single crystals. For any orientation of the sample with respect to the x-ray beam, the pre-edge peak grows and shifts to lower energy with temperature. In addition temperature induces modifications in the position and intensities of the main XANES features. First-principles DFT calculations are performed for both compounds. They show that the pre-edge peak originates from forbidden 1s to 3s transitions induced by vibrations. Three existing theoretical models are used to take vibrations into account in the absorption cross section calculations: i) an average of the XANES spectra over the thermal displacements of the absorbing atom around its equilibrium position, ii) a method based on the crude Born-Oppenheimer approximation where only the initial state is averaged over thermal displacements, iii) a convolution of the spectra obtained for the atoms at the equilibrium positions with an approximate phonon spectral function. The theoretical spectra so obtained permit to qualitatively understand the origin of the spectral modifications induced by temperature. However the correct treatment of thermal fluctuation in XANES spectroscopy requires more sophisticated theoretical tools

High-pressure study of X-ray diffuse scattering in ferroelectric perovskites

We present a high-pressure x-ray diffuse scattering study of the ABO$_3$ ferroelectric perovskites BaTiO_3 and KNbO_3. The well-known diffuse lines are observed in all the phases studied. In KNbO_3, we show that the lines are present up to 21.8 GPa, with constant width and a slightly decreasing intensity. At variance, the intensity of the diffuse lines observed in the cubic phase of BaTiO_3 linearly decreases to zero at $\sim 11$ GPa. These results are discussed with respect to x-ray absorption measurements, which leads to the conclusion that the diffuse lines are only observed when the B atom is off the center of the oxygen tetrahedron. The role of such disorder on the ferroelectric instability of perovskites is discussed.Comment: 4 pages, Accepted in PR

Study of the Galactic Interstellar Medium from High Resolution X-Ray Spectroscopy: X-Ray Absorption Fine Structure and Abundances of O, Mg, Si, S, and Fe

We study the composition of the Galactic interstellar medium (ISM) toward the Galactic center region (5 < |l| < 20 degree) by utilizing X-ray absorption features of three bright low-mass X-ray binaries (LMXBs), GX 13+1, GX 5-1, and GX 340+0, observed with the Chandra HETGS. We detect X-ray absorption fine structure (XAFS) of the Si K-edge, characterized by a narrow and a broad absorption feature at 1846 and ~1865 eV, respectively. Comparison with ground experimental data indicates that most of the ISM Si exists in the form of silicates, although a composition of "pure" forsterite is ruled out. The XAFS spectra of the sulfur K-edge indicate that a significant fraction of S exists in the gas phase. From each source, we derive the column densities of Mg, S, Si, and Fe from the K-edge depth and that of O (or H) from the absorption of the continuum. The elemental abundance ratios are found to be consistent between the three targets: the mean values of O/Si, Mg/Si, S/Si, and Fe/Si are determined to be 0.55+-0.17, 1.14+-0.13, 1.03+-0.12, and 0.97+-0.31 solar, respectively (90% error in the mean value). We discuss the origins of the overabundances of the heavy metals relative to O in the Galactic ISM by comparison with the abundance pattern of the intracluster medium in clusters of galaxies. Assuming that most of the Mg and Si atoms are depleted into silicates of either the proxine or olivine family, we estimate that the number ratio of Mg to Fe in olivine is >~1.2 and that 17%-43% of the total O atoms in the ISM must be contained in silicate grains.Comment: 31 pages, 15 figures, accepted for publication in ApJ, vol. 620, 2005. Proof corrections are reflected (column densities of O and H were overestimated in the previous version.). Figures 1(a)-(c) are revise

Influence of the 6^1S_0-6^3P_1 Resonance on Continuous Lyman-alpha Generation in Mercury

Continuous coherent radiation in the vacuum-ultraviolet at 122 nm (Lyman-alpha) can be generated using sum-frequency mixing of three fundamental laser beams in mercury vapour. One of the fundamental beams is at 254 nm wavelength, which is close to the 6^1S_0-6^3P_1 resonance in mercury. Experiments have been performed to investigate the effect of this one-photon resonance on phasematching, absorption and the nonlinear yield. The efficiency of continuous Lyman-alpha generation has been improved by a factor of 4.5.Comment: 8 pages, 7 figure

X-ray Absorption Near-Edge Structure calculations with pseudopotentials. Application to K-edge in diamond and alpha-quartz

We present a reciprocal-space pseudopotential scheme for calculating X-ray absorption near-edge structure (XANES) spectra. The scheme incorporates a recursive method to compute absorption cross section as a continued fraction. The continued fraction formulation of absorption is advantageous in that it permits the treatment of core-hole interaction through large supercells (hundreds of atoms). The method is compared with recently developed Bethe-Salpeter approach. The method is applied to the carbon K-edge in diamond and to the silicon and oxygen K-edges in alpha-quartz for which polarized XANES spectra were measured. Core-hole effects are investigated by varying the size of the supercell, thus leading to information similar to that obtained from cluster size analysis usually performed within multiple scattering calculations.Comment: 11 pages, 4 figure

Quadrupole moment of the 6− isomeric state in 66Cu: Interplay between different nuclear deformation driving forces

AbstractWe have measured the spectroscopic quadrupole moment of the 6− isomeric state in 66Cu to be |Qs|=18.6(12) efm2. This state results from a weak coupling of the πp3/2 and the νg9/2 orbitals, which lead to sizable deformation at oblate and prolate shapes, correspondingly, in the 68Ni region. The interplay between these two different deformation-driving orbitals is observed at N=37 for the 6− state resulting in a most probable oblate shape

Deformation change in light iridium nuclei from laser spectroscopy

Laser spectroscopy measurements have been performed on neutron-deficient and stable Ir isotopes using the COMPLIS experimental setup installed at ISOLDE-CERN. The radioactive Ir atoms were obtained from successive decays of a mass-separated Hg beam deposited onto a carbon substrate after deceleration to 1kV and subsequently laser desorbed. A three-color, two-step resonant scheme was used to selectively ionize the desorbed Ir atoms. The hyperfine structure (HFS) and isotope shift (IS) of the first transition of the ionization path 5d^{7}6s ^{2}^{4}F_{9/2} \to 5d^{7}6s6p ^{6}F_{11/2} at 351.5nm were measured for $^{182-189}$Ir, $^{186}Ir^{m}$ and the stable $^{191,193}$Ir. The nuclear magnetic moments μI and the spectroscopic quadrupole moments Qs were obtained from the HFS spectra and the change of the mean square charge radii from the IS measurements. The sign of μI was experimentally determined for the first time for the masses 182≤A≤189 and the isomeric state $^{186}Ir^ m$ . The spectroscopic quadrupole moments of $^{182}$Ir and $^{183}$Ir were measured also for the first time. A large mean square charge radius change between $^{187}$Ir and $^{186}Ir^g$ and between $^{186}Ir^m$ and $^{186}Ir ^g$ was observed corresponding to a sudden increase in deformation: from β2 ≃ + 0.16 for the heavier group A = 193, 191, 189, 187 and 186m to β2 ≥ + 0.2 for the lighter group A = 186g, 185, 184, 183 and 182. These results were analyzed in the framework of a microscopic treatment of an axial rotor plus one or two quasiparticle(s). This sudden deformation change is associated with a change in the proton state that describes the odd-nuclei ground state or that participates in the coupling with the neutron in the odd-odd nuclei. This state is identified with the π3/2+[402] orbital for the heavier group and with the π1/2-[541] orbital stemming from the 1h _9/2 spherical subshell for the lighter group. That last state seems to affect strongly the observed values of the nuclear moments

Prospects for measuring the gravitational free-fall of antihydrogen with emulsion detectors

The main goal of the AEgIS experiment at CERN is to test the weak equivalence principle for antimatter. AEgIS will measure the free-fall of an antihydrogen beam traversing a moir\'e deflectometer. The goal is to determine the gravitational acceleration g for antihydrogen with an initial relative accuracy of 1% by using an emulsion detector combined with a silicon micro-strip detector to measure the time of flight. Nuclear emulsions can measure the annihilation vertex of antihydrogen atoms with a precision of about 1 - 2 microns r.m.s. We present here results for emulsion detectors operated in vacuum using low energy antiprotons from the CERN antiproton decelerator. We compare with Monte Carlo simulations, and discuss the impact on the AEgIS project.Comment: 20 pages, 16 figures, 3 table

Annihilation of low energy antiprotons in silicon

The goal of the AE$\mathrm{\bar{g}}$IS experiment at the Antiproton Decelerator (AD) at CERN, is to measure directly the Earth's gravitational acceleration on antimatter. To achieve this goal, the AE$\mathrm{\bar{g}}$IS collaboration will produce a pulsed, cold (100 mK) antihydrogen beam with a velocity of a few 100 m/s and measure the magnitude of the vertical deflection of the beam from a straight path. The final position of the falling antihydrogen will be detected by a position sensitive detector. This detector will consist of an active silicon part, where the annihilations take place, followed by an emulsion part. Together, they allow to achieve 1$$ precision on the measurement of $\bar{g}$ with about 600 reconstructed and time tagged annihilations. We present here, to the best of our knowledge, the first direct measurement of antiproton annihilation in a segmented silicon sensor, the first step towards designing a position sensitive silicon detector for the AE$\mathrm{\bar{g}}$IS experiment. We also present a first comparison with Monte Carlo simulations (GEANT4) for antiproton energies below 5 MeVComment: 21 pages in total, 29 figures, 3 table