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The double K-shell ionization of Sc, Cr and Cu induced by electron impact was investigated via high energy resolution measurements of the Kα diagram transitions and the transitions resulting from the radiative decay of K-shell double vacancy states, namely the Khα hypersatellites. For Sc, the Kβ diagram lines and Khβ hypersatellites were also measured. The measurements were carried out in-house with a von Hamos curved crystal spectrometer operated in the so-called direct geometry in which the anodes of Sc, Cr and Cu X-ray tubes were used as targets. For each element, the electron kinetic energy was chosen to be about twice the threshold energy for the double 1s ionization. The double-to-single ionization cross-sections ratios PKK were deduced from the hypersatellite-to-diagram line yield ratios, corrected beforehand for the self-absorption of the X-rays in the target and the energy dependent efficiency of the spectrometer. The obtained ratios are discussed and compared to other PKK values found in the literature for electrons and photons.

We report on the radiative decay of double $K$-shell vacancy states produced in solid Ca, V, Fe, and Cu targets by impact with about 10 MeV/amu C and Ne ions. The resulting $K$ hypersatellite x-ray emission spectra were measured by means of high-energy-resolution spectroscopy using a von Hamos bent crystal spectrometer. The experiment was carried out at the Philips variable energy cyclotron of the Paul Scherrer Institute. From the fits of the x-ray spectra the energies, line widths, and relative intensities of the hypersatellite x-ray lines could be determined. The fitted intensities were corrected to account for the energy-dependent solid angle of the spectrometer, effective source size, target self-absorption, crystal reflectivity, and detector efficiency. The single-to-double $K$-shell ionization cross-section ratios were deduced from the corrected relative intensities of the hypersatellites and compared to theoretical predictions from the semiclassical approximation model using hydrogenlike and Dirac-Hartree-Fock wave functions and from classical trajectory Monte Carlo calculations.

International audience; The x-ray atomic properties of nickel (Ni) were investigated in a unique approach combining different experimental techniques to obtain new, useful and reliable values of atomic fundamental parameters for x-ray spectrometric purposes and for comparison with theoretical predictions. We determined the mass attenuation coefficients in an energy range covering the L-and K-absorption edges, the K-shell fluorescence yield and the $K\beta$ / $K\alpha$ and $K\beta_{1,3}$/$K\alpha_{1,2}$ transition probability ratios. The obtained line profiles and linewidths of the $K\alpha$ and $K\beta$ transitions in Ni can be considered as the contribution of the satellite lines arising from the [KM] shake processes suggested by Deutsch et al (1995 Phys. Rev. A 51 283) and Ito et al (2016 Phys. Rev. A 94 042506). Comparison of the new data with several databases showed good agreement, but also discrepancies were found with existing tabulated values.

The potential of valence to core Al X-ray emission spectroscopy to determine aluminum distribution in ferrierite zeolites was investigated. The recorded emission spectra of four samples prepared with different structure directing agents exhibit slight variations in the position of the main emission peak and the intensity of its low energy shoulder. Theoretical calculations indicate that an increased intensity of the Kβx shoulder in the Al emission spectra can be linked to a predominant occupation of the T3 site by a single aluminum atom. This study thus suggests that valence to core X-ray emission spectroscopy can be applied to help determine the occupation of aluminum at crystallographic T-sites in zeolites.

We report on a laboratory-based facility for in-house x-ray absorption fine structure (XAFS) measurements. The device consists of a conventional x-ray source for the production of the incident polychromatic radiation and a von Hamos bent crystal spectrometer for the analysis of the incoming and transmitted radiation. The reliability of the laboratory-based setup was evaluated by comparing the Cu K-edge and Ta L3- edge XAFS spectra obtained in-house with the corresponding spectra measured at a synchrotron radiation facility. To check the accuracy of the device, the K- and L-edge energies and the attenuation coefficients below and above the edges of several 3d, 4d, and 5d elements were determined and compared with the existing experimental and theoretical data. The dependence of the XAFS spectrum shape on the oxidation state of the sample was also probed by measuring inhouse the absorption spectra of metallic Fe and two Fe oxides (Fe2O3 and Fe3O4).

The design and performance of a high-resolution transmission-type X-ray spectrometer for use in the 15-26 keV energy range at synchrotron light sources is reported. Monte Carlo X-ray-tracing simulations were performed to optimize the performance of the transmission-type spectrometer, based on the DuMond geometry, for use at the Super X-ray absorption beamline of the Swiss Light Source at the Paul Scherrer Institute. This spectrometer provides an instrumental energy resolution of 3.5 eV for X-ray emission lines around 16 keV and 12.5 eV for emission lines at 26 keV, which is comparable to the natural linewidths of the K and L X-ray transitions in the covered energy range. First experimental data are presented and compared with results of the Monte Carlo X-ray simulations.

The grazing emission X-ray fluorescence (GEXRF) technique was applied to the analysis of different Al films, with nominal thicknesses in the range of 1 nm to 150 nm, on Si wafers. In GEXRF the sample volume from which the fluorescence intensity is detected is restricted to a near-surface region whose thickness can be tuned by varying the observation angle. This is possible because of the refraction of the fluorescence X-rays and the quite long emission paths within the probed sample. By recording the X-ray fluorescence signal for different shallow emission angles, defined relatively to the flat, smooth sample surface, the deposited Al surface layers of the different samples could be well characterized in terms of layer thickness, layer density, oxidation and surface roughness. The advantages offered by synchrotron radiation and the employed wavelength-dispersive detection setup were profited from. The GEXRF results retrieved were confirmed by complementary measurements. The experimental setup, the principles and advantages of GEXRF and the analysis of the recorded angular intensity profiles will be discussed in details.

We report on vacuum ultraviolet (VUV) excited photoluminescence (PL) spectra emitted from a chemical vapor deposited MoS2 few-layered film. The excitation spectrum was recorded by monitoring intensities of PL spectra at ~1.9 eV. A strong wide excitation band peaking at 7 eV was found in the excitation. The PL excitation band is most intensive at liquid helium temperature and completely quenched at 100 K. Through first-principles calculations of photoabsorption in MoS2, the excitation was explicated and attributed to transitions of electrons from p- and d- type states in the valence band to the d- and p-type states in the conduction band. The obtained photon-in/photon-out results clarify the excitation and emission behavior of the low dimensional MoS2 when interacting with the VUV light sources.

We report on the surface-sensitive grazing emission X-ray fluorescence technique combined with synchrotron radiation excitation and high-resolution detection to realize depth-profile measurements of Al-implanted Si wafers. The principles of grazing emission measurements as well as the benefits offered by synchrotron sources and wavelength-dispersive detection setups are presented. It is shown that the depth distribution of implanted ions can be extracted from the dependence of the X-ray fluorescence intensity on the grazing emission angle with nanometer-scale precision provided that an analytical function describing the shape of the depth distribution is assumed beforehand. If no a priori assumption is made, except a bell shaped form for the dopant distribution, the profile derived from the measured angular distribution is found to reproduce quite satisfactorily the depth distribution of the implanted ions. Copyright © 2012 John Wiley & Sons, Ltd.

The synchrotron radiation based high-resolution grazing emission X-ray fluorescence (GEXRF) technique was used to extract the distribution of Al ions implanted with a dose of 1016 atoms/cm2 in Si wafers with energies ranging between 1 and 100 keV. The depth distributions of the implanted ions were deduced from the measured angular profiles of the Al-Kα X-ray fluorescence line with nanometer-scale precision. The experimental results were compared to theoretical predictions of the depth distributions resulting from ion implantation. A good agreement between experiment and theory was found which proved that the presented high-resolution grazing emission X-ray fluorescence technique is well suited to perform depth profiling measurements of impurities located within the extinction depth, provided the overall shape of the distribution can be assumed a priori.

High-resolution measurements of the photoinduced X-ray emission of liquid mercury were performed, using a transmission DuMond-type crystal spectrometer for transitions above 11 keV and a reflection von Hamos-type crystal spectrometer for transitions below 11 keV. The target X-ray fluorescence was produced by irradiating the sample with the Bremsstrahlung from X-ray tubes. The energies and natural linewidths of 6 K-shell, 26 L-shell and 2 M-shell X-ray transitions were determined. Using a least-squares-fit method to solve the two sets of equations derived from the observed transition energies and transition widths the binding energies of the subshells K to M₅ and O₁ and the level widths of the subshells K to N₅ and O₁ could also be determined.

We report on the investigation of the photon energy dependence of double 1s photoionization of light atoms and compare the cross sections for hollow atom and He-like ion production. Measurements of the Kα hypersatellite x-ray spectra of Mg, Al, and Si were carried out using the Fribourg high-resolution x-ray spectrometer installed at the ID21 and ID26 beam lines at the ESRF. The double-to-single photoionization cross section ratios were derived as a function of the incident photon beam energy and compared to convergent close-coupling (CCC) calculations for He-like ions. The dynamical electron-electron scattering contribution to the DPI cross-sections was found to be more important for neutral atoms than for the He isoelectronic series.

We report the results of the x-ray radiative recombination (RR) experiment at the electron cooler of the ESR storage ring performed, for the first time, for detuned (off-cooling) electron energies. In this experiment the recombination of stored, decelerated bare uranium ions with electrons in the energy range 0–1000 meV was studied by observing K-RR x-ray photons emitted from direct radiative recombination to the lowest n=1 state. In this way the RR process was studied in a state selective manner for several off-cooling electron energies. The measured dependency of the recombination rate on the relative electron energies for K-shell RR x-ray photons are compared with the predictions of both nonrelativistic and fully relativistic calculations for the radiative recombination. A role of the relativistic effects, which contribute substantially for higher relative electron energies, are discussed. Strong enhancement of the recombination rate is observed for the the zero relative electron energy (cooling condition) for the K-shell.

In this work our previous study about chemical effects in the Kα spectra of S compounds employing high-resolution X-ray spectroscopy has been extended to the Kβ emission spectra. The measurements were performed with a wavelength dispersive single crystal spectrometer operated in the von Hamos geometry having an energy resolution comparable to the natural linewidth of the measured Kβ X-ray lines. The target fluorescence was produced by irradiating the samples with the bremsstrahlung from an X-ray tube. The energies and widths of the main components in the Kβ emission spectrum are given for different sulfur compounds (sulfide, sulfite, sulfate). The measured energy shifts between the Kβ lines of the compounds and elemental sulfur are presented as a function of the sulfur oxidation state and compared with the results obtained from the former Kα measurements.

Fluorescence yields (FYs) for the Ge $L$ shell were determined by a theoretical and two experimental groups within the framework of the International Initiative on X-Ray Fundamental Parameters Collaboration. Calculations were performed using the Dirac-Fock method, including relativistic and QED corrections. The experimental value of the ${L}_{3}\phantom{\rule{0.28em}{0ex}}\mathrm{FY}\phantom{\rule{0.28em}{0ex}}{\ensuremath{\omega}}_{{L}_{3}}$ was determined at the Physikalisch-Technische Bundesanstalt undulator beamline of the synchrotron radiation facility BESSY II in Berlin, Germany, and the $L{\ensuremath{\alpha}}_{1,2}$ and $L{\ensuremath{\beta}}_{1}$ line widths were measured at the Swiss Light Source, Paul Scherrer Institute, Switzerland, using monochromatized synchrotron radiation and a von Hamos x-ray crystal spectrometer. The measured fluorescence yields and line widths are compared to the corresponding calculated values.

The high-resolution von Hamos Bragg crystal spectrometer was constructed for the study of K X-ray emission from low- Z elements and L and M X-ray spectra of medium to high Z elements. Recently, this instrument was applied to high-resolution XES and RIXS studies using X-ray synchrotron radiation at the ID21 and BM5 beamlines at the ESRF. An outline of the spectrometer design and performance characteristics will be given. The studies deal with the energy dependent KL double photoexcitation of argon, the L 3 and M 1 atomic-level widths of elements 54≤ Z ≤77, and the evolution of the K-edge RIXS spectra of manganese oxides.

The high-resolution spectra of thorium Mα 1,2 (M 5 N 6,7 ) and Mβ(M 4 N 6 ) X-ray lines induced by O and Ne ions with energies 376 and 178 MeV, respectively, have been measured using a von Hamos crystal spectrometer. The measured spectra exhibit the pronounced X-ray satellite structure due to the multiple ionization in the N- and M-shells. In particular the N-shell satellites are well resolved and the M-shell hypersatellites are clearly observed, to the best of our knowledge, for the first time. The observed M-X-ray diagram transitions and their satellites are interpreted using the multi-configuration Dirac-Fock (MCDF) calculations performed for the multi-vacancy configurations including up to two spectator vacancies. The comparison shows that calculations for more vacancies are needed to reproduce the measured X-ray structure. On the other hand, the data are well interpreted qualitatively using a simplified model of the “average” MCDF satellites having binomially distributed intensities. Further MCDF calculations are in the progress, which ultimately allow to extract precise (∼0.5 eV) information on the electronic structure of the multiple ionized thorium.

The Kβ spectrum of 42Mo bombarded by 20.8 MeV/amu carbon ions was measured with high-resolution using a transmission-type bent crystal spectrometer operated in the modified DuMond slit geometry. The M-shell satellites of the Kβ2 transition could be well resolved, whereas for the Kβ1,3 transitions only a broadening and shift of the line centroid was observed. The composite structure of the satellite lines which consist of many components that vary in energy and strength was analyzed using theoretical energies and relative intensities obtained from multiconfiguration Dirac–Fock calculations. From the data analysis average M-shell satellite-to-diagram line yield ratios were deduced for both the Kβ1,3 and Kβ2 transitions. For the Kβ2 transition for which the relative contributions of the 3s,p and 3d spectator vacancies to the observed Kβ2M1 satellite yield could be determined, separated X(Kβ2M11,2,3):X(Kβ2M0) and X(Kβ2M14,5):X(Kβ2M0) yield ratios could even be extracted.

High-resolution measurements of the Kα x-ray spectra of metallic Ca, Ti, Cr and Fe were performed with a von Hamos Bragg crystal spectrometer. The target x-ray emission was induced by 34, 72 and 134 MeV C ions, 28, 64 and 230 MeV O ions and 43, 160 and 380 MeV Ne ions. The energies of the resolved KαLN x-ray satellite lines were determined. The possible variation of the energy differences between neighboring KαLN lines with the projectile energy, projectile atomic number and number of target L shell spectator vacancies was probed. No significant dependence on the projectile characteristics was observed. In contrast, the absolute energies of the KαLN satellite lines were found to depend on the projectile velocity. This dependence was attributed to the additional M shell ionization of the target atoms. Copyright © 2003 John Wiley & Sons, Ltd.

In this work two synchrotron radiation-based depth-sensitive X-ray fluorescence techniques, grazing incidence X-ray fluorescence (GIXRF) and grazing emission X-ray fluorescence (GEXRF), are compared and their potential for non-destructive depth-profiling applications is investigated. The depth-profiling capabilities of the two methods are illustrated for five aluminum-implanted silicon wafers all having the same implantation dose of 1016 atoms per cm2 but with different implantation energies ranging from 1 keV up to 50 keV. The work was motivated by the ongoing downscaling effort of the microelectronics industry and the resulting need for more sensitive methods for the impurity and dopant depth-profile control. The principles of GIXRF and GEXRF, both based on the refraction of X-rays at the sample surface to enhance the surface-to-bulk ratio of the detected fluorescence signal, are explained. The complementary experimental setups employed at the Physikalisch-Technische Bundesanstalt (PTB) for GIXRF and the University of Fribourg for GEXRF are presented in detail. In particular, for each technique it is shown how the dopant depth profile can be derived from the angular intensity dependence of the Al Kα fluorescence line. The results are compared to theoretical predictions and, for two samples, crosschecked with values obtained from secondary ion mass spectroscopy (SIMS) measurements. A good agreement between the different approaches is found proving that the GIXRF and GEXRF methods can be efficiently employed to extract the dopant depth distribution of ion-implanted samples with good accuracy and over a wide range of implantation energies.

photoexcitation spectra. Both two-electron excitation spectra are well described by a model spectrum builtofconsecutivebound-bounddiscretetransitionsandshake-upandshake-offchannelsgivingpreciseenergiesandintensitiesofthecorrespondingcontributions.Theobtainedresultsarecomparedwithotherexistingexperimentalvalues based on x-ray-absorption measurements and theoretical predictions.DOI: 10.1103/PhysRevA.90.022513 PACS number(s): 32

The high-resolution von Hamos bent crystal spectrometer of the University of Fribourg was upgraded with a focused X-ray beam source with the aim of performing micro-sized X-ray fluorescence (XRF) measurements in the laboratory. The focused X-ray beam source integrates a collimating optics mounted on a low-power micro-spot X-ray tube and a focusing polycapillary half-lens placed in front of the sample. The performances of the setup were probed in terms of spatial and energy resolution. In particular, the fluorescence intensity and energy resolution of the von Hamos spectrometer equipped with the novel micro-focused X-ray source and a standard high-power water-cooled X-ray tube were compared. The XRF analysis capability of the new setup was assessed by measuring the dopant distribution within the core of Er-doped SiO2 optical fibers.

X-ray emission spectra recorded in the off-resonant regime carry information on the density of unoccupied states. It is known that by employing the Kramers-Heisenberg formalism, the high energy resolution off-resonant spectroscopy (HEROS) is equivalent to the x-ray absorption spectroscopy (XAS) technique and provides the same electronic state information. Moreover, in the present Letter we demonstrate that the shape of HEROS spectra is not modified by self-absorption effects. Therefore, in contrast to the fluorescence-based XAS techniques, the recorded shape of the spectra is independent of the sample concentration or thickness. The HEROS may thus be used as an experimental technique when precise information about specific absorption features and their strengths is crucial for chemical speciation or theoretical evaluation.

X-ray and UV photons were used to store xenon atoms in polymeric films. The trapping was found to be stable at room temperature for Kapton and PVDC films. In Kapton, concentrations of xenon up to about 18.5 mg/cm3 were attained. The dependence of the rare gas concentration on the irradiation dose, film thickness, gas pressure, and on the polymers and gases nature was probed. The results are interpreted in terms of a simple three-step model: the xenon atoms are first physisorbed at the surface of the substrate and then diffuse into the bulk where they are finally trapped as a result of radiation chemistry effects of the UV or X-rays on the structure of the polymer.

We report on the study of heavy-ion-induced Si KL x-ray satellite spectra of several 3d, 4d and 5d silicides, with the aim of elucidating the trends in bonding properties of transition metal (TM) silicides. Measurements of the 43 MeV Ne3+-beam-induced Si KL spectra of elemental silicon and compound targets were performed at the Paul Scherrer Institute, Villigen, Switzerland, with a high-resolution von Hamos crystal spectrometer. The interpretation of the data was based on the importance of the effect of the solid and chemical environment on the KL x-ray satellite relative intensities due to the L-vacancy refilling by intra- and inter-atomic electron transitions. Within the framework of a statistical procedure for L-shell vacancy refilling the average L-shell rearrangement probability for each silicide was extracted so that calculated x-ray intensity distributions matched the experimental ones. The results are discussed in terms of the interplay of Si-Si, Si-TM and TM-TM bonding interactions in the studied TM silicides.

High-resolution measurements of the Kα 1,2 X-ray spectra were performed with a bent crystal diffraction spectrometer for zirconium, niobium, molybdenum and palladium targets bombarded by 280 and 360 MeV oxygen ions. The energy differences between the Kα 1,2 diagram and the K h α 1,2 hypersatellite transitions as well as the intensity ratios I ( K h α 1 )/ I ( K h α 2 ) were determined. The L-shell satellites of the diagram and of the hypersatellite lines were resolved. The data are interpreted in terms of the properties of He-like hole states in mid- Z atoms. The Breit interaction correction is determined. The corrections due to the unresolved M-shell satellites and to the QED are found to be much smaller than the Breit terms and comparable to the experimental accuracy.

A new technique which allows the storage of noble gases in polymeric films at ambient temperature was successfully developed. The trapping of the rare gases in the polymer takes place via X-ray irradiation of the gas and the polymer film by means of an X-ray tube. Concentrations up to about 2 × 1017 atoms of noble gas per cm2 of the film were obtained. The thermal energy needed for desorbing Xe from a kapton film was found to be about 16 kcal/mol which is large compared with the known values for thermal desorptions on metal surfaces. An energy shift of 1.04 ± 0.48 eV was further observed for the 5p–1s X-ray transition of trapped Xe atoms, which permits to surmise a rather strong interaction between the sorbate atoms and the sorbent molecules. Two interpretations of the observed phenomena are presented, the first involves bond ruptures and bond rearrangements in the polymer whereas the second is based on the assumption that chemisorption or persorption of Xe occurs in the polymeric substrate.

The K–LM radiative Auger (RA) x-ray spectrum of argon was observed. The transitions were photoinduced by means of an x-ray tube and measured with two different high-resolution curved crystal spectrometers of reflection-type geometry. From the first measurements performed at the Paul Scherrer Institute (PSI), only an upper limit of 0.25% relatively to the intensity of the Kα1,2 diagram line could be obtained for the total K—LM RA yield. From a second experiment carried out at the University of Fribourg, a I(K–LM RA)/I(Kα1,2) ratio of 0.18±0.05% was obtained. This value is consistent with the PSI result but in strong disagreement with theoretical predictions based on the shake model, which are about four times larger. © 1998 John Wiley & Sons, Ltd.

The photoinduced $K\ensuremath{\alpha}$ and $K\ensuremath{\beta}$ x-ray spectra of argon and krypton were measured by means of high-resolution crystal diffractometry. Ar $K{\ensuremath{\alpha}}_{1,2}{L}^{(1)}$ and $K{\ensuremath{\beta}}_{1,3}{M}^{(1,2)}$ and Kr $K{\ensuremath{\alpha}}_{1}{L}^{(1)}$ and $K{\ensuremath{\beta}}_{2}{M}^{(1,2)}$ satellites were observed and resolved from the corresponding diagram lines. From the satellite to parent diagram line yield ratios, the probabilities for producing via shake processes ${K}^{(1)}{L}^{(1)}$ and ${K}^{(1)}{M}^{(1)}$ double-hole states were deduced. The results are compared to the few other existing experimental data and to theoretical sudden approximation predictions. The latter are found to underestimate somewhat the experimental values.

We report on a high-resolution transmission-type curved crystal spectrometer based on the modified DuMond slit geometry. The spectrometer was developed at the University of Fribourg for the study of photoinduced X-ray spectra. K and L X-ray transitions with energies above about 10 keV can be measured with an instrumental resolution comparable to their natural linewidths. Construction details and operational characteristics of the spectrometer are presented. The variation of the energy resolution as a function of the focal distance and diffraction order is discussed. The high sensitivity of the spectrometer is demonstrated via the 2s-1s dipole-forbidden X- ray transition of Gd which could be observed despite its extremely low intensity. The precision of the instrument is illustrated by comparing the sum of the energies of the Au K–L 2 and L 2–M 3 cascading transitions with the energy of the crossover K–M 3 transition as well as by considering the energy differences of the Gd Kα1 X-ray line measured at five different diffraction orders. Finally, to demonstrate the versatility of the spectrometer, it is shown that the latter can also be used for in-house extended X- ray absorption fine structure measurements.

M. Czarnota,1,* D. Banaś,1 M. Berset,2 D. Chmielewska,3 J.-Cl. Dousse,2 J. Hoszowska,2 Y.-P. Maillard,2 O. Mauron,2 M. Pajek,1 M. Polasik,4 P. A. Raboud,2 J. Rzadkiewicz,5 K. Slabkowska,4 and Z. Sujkowski3,† 1Institute of Physics, Jan Kochanowski University, 25-406 Kielce, Poland 2Department of Physics, University of Fribourg, CH-1700 Fribourg, Switzerland 3Soltan Institute for Nuclear Studies, 05-400 Otwock-Świerk, Poland 4Faculty of Chemistry, Nicholas Copernicus University, 87-100 Torun, Poland 5National Centre for Nuclear Research, 05-400 Otwock-Świerk, Poland (Received 15 June 2013; published 11 November 2013)

A high-resolution von Hamos Bragg crystal X-ray spectrometer is described. The instrument was designed for the study of X-ray emission from low-Z elements and L X-ray spectra of medium to high Z targets induced by photon and particle impact. The construction details and operational characteristics of the spectrometer are presented along with the data illustrating the utility of this facility in different areas of research in atomic physics.

The influence of solid and chemical effects on photo-induced x-ray transitions from the valence states was investigated by means of high-resolution x-ray diffractometry. The study was devoted to metallic Mo and , and compounds. A significant enhancement of the emission rate of the 4d - 1s and 4d - 2s quadrupole-allowed transitions was found for the targets studied. The change of the transition probability is interpreted as being due to the mixing of the 4d states with p character orbitals. Further, the effect of exchange interaction between the 4p core level and the

High-resolution measurements of the K{beta}{sub 2} diagram line and its M{sup 1} satellite were performed for zirconium, molybdenum, palladium, and praseodymium. The x-ray spectra were induced by impact with 28-, 40-, 65-, and 100-MeV {alpha} particles and measured with a transmission-type bent crystal spectrometer in modified DuMond slit geometry. From the relative yields of the K{beta}{sub 2}M{sup 1} satellites the experimental average M-shell ionization probabilities for nearly central collisions were deduced. They are compared with theoretical predictions from the semiclassical independent particle approximation using either hydrogenlike wave functions (SCA-HWF) or Dirac-Hartree-Fock wave functions (SCA-DHF), pointing out the relevance of the use of DHF wave functions instead of hydrogenlike wave functions in the SCA model. Moreover, the experimental energy shifts of the satellite transitions with respect to the diagram lines are compared to results of extensive multiconfiguration Dirac-Fock calculations. {copyright} {ital 1998} {ital The American Physical Society}

Excited levels of the strongly-deformed odd-odd nucleus 166Tm, populated by the 165Ho(α,3nγ) reaction, were investigated using standard in-beam γ-ray spectroscopy, including measurements of a few conversion electron lines, and by high-resolution curved-crystal spectroscopy. A level scheme consisting of 178 transitions among 6 well-developed and 4 partial rotational bands is proposed. Level spins and parities were determined and the results were interpreted in the framework of the Nilsson model by comparison with predictions. The Gallagher-Moszkowski splitting for the { π 1 2 + [411] ± ν 5 2 + [642] } configuration was determined to be 245(20) keV. An anomalous signature splitting was observed for the {π 7 2 + [404] + ν 5 2 + [642]}K π = 6 + configuration.

We report on the design and performance of a wavelength-dispersive type spectrometer based on the von Hamos geometry. The spectrometer is equipped with a segmented-type crystal for x-ray diffraction and provides an energy resolution in the order of 0.25 eV and 1 eV over an energy range of 8000 eV–9600 eV. The use of a segmented crystal results in a simple and straightforward crystal preparation that allows to preserve the spectrometer resolution and spectrometer efficiency. Application of the spectrometer for time-resolved resonant inelastic x-ray scattering and single-shot x-ray emission spectroscopy is demonstrated.

The mechanisms leading to the production of hollow K shell atoms via single photon impact were investigated for a variety of light elements with 12 ≤ Z ≤ 23. The double 1s vacancy states were produced by irradiating the samples with intense monoenergetic synchrotron radiation beams. The double-to-single K-shell photoionization probabilities PKK and the absolute double K-shell photoionization cross sections σ²⁺ were determined by measuring with a high-resolution bent von Hamos crystal spectrometer the Kαh hypersatellite X-ray emission of the samples. The measurements were performed over a wide range of incoming photon energies from threshold up to energies beyond the broad maximum of the double-to-single photoionization cross section ratios. The PKK and σ²⁺ were determined from the relative yields of the resolved Kαh hypersatellite lines. For Mg, Al and Si, the two-electron one-photon (TEOP) Kααh transitions which represent an alternative but much weaker decay channel for double 1s vacancy states could be also observed, using a highly efficient flat crystal wavelength dispersive spectrometer. This observation of single photon-induced TEOP transitions has shown that the I(Kαh)/I(Kααh) branching ratios are very poorly reproduced by most of existing theoretical models. Besides the relative yields of the hypersatellite and TEOP transitions, the energies and natural linewidths of the Kαh and Kααh X-ray lines were also determined. The energies are found to be in good agreement with different theoretical predictions, whereas the linewidths are significantly underestimated by the calculations, except if non-lifetime broadening effects such as the outer-shell ionization and the open valence configuration are taken into consideration.

The KMM radiative Auger (RA) x-ray spectra of solid Ca were induced by monochromatic synchrotron radiation and measured with a high-resolution von Hamos bent crystal spectrometer. Two excitation energies were employed, one in the near K threshold region and the second well above the K absorption edge. The KMM RA spectral structure and relative intensity with respect to the diagram K{beta}{sub 1,3} (K-M{sub 3,2}) line are found to be independent of the excitation energy. The overall RA structure resembles the density of unoccupied s, p, and d states. Due to solid-state effects, however, spectral features resulting from the major discrete shake-up transitions could not be resolved. For the total KMM RA to K{beta}{sub 1,3} yield ratio, a value of 0.053(3) is obtained. The latter is compared to theoretical predictions and available experimental data obtained by various types of target excitation.

The electron-induced ${L}_{3}M$ two-step double ionization cross sections of metallic Pd were determined experimentally for incident electron beam energies ranging from the double ionization threshold up to 18 keV. The double ${L}_{3}M$ ionization cross sections were derived from the intensity ratios (${I}_{L\ensuremath{\alpha}M}$:${I}_{L\ensuremath{\alpha}}$) of the resolved $M$ satellites to the parent diagram lines. The sample was bombarded with monoenergetic electrons from an energy-tunable 20-kV electron gun. The diagram and $M$-satellite x-ray lines were measured by means of high-resolution x-ray spectroscopy, using a reflection-type von Hamos bent crystal spectrometer. The two-step partial cross sections were determined by subtracting from the measured total double ionization cross sections the contributions due to the shake process and ${L}_{1}$-${L}_{3}{M}_{4,5}$ Coster-Kronig transitions. Despite the thick target employed in the present study, the dependence of the two-step cross sections on the incoming electron energy could be derived using a target slice decomposition method. It is shown that the obtained energy dependence can be well reproduced by the semiempirical parametrization model of Pattard and Rost.

The first experimental results of a high-resolution study of Th and U Lγ-X-rays induced in collisions with 230 MeV and 360 MeV oxygen ions, undertaken to investigate the dynamics of the multiple ionization in M-, N- and O-shells and the structure of M- and N-shell X-ray satellites, are reported. The measurements were performed using the transmission curved- crystal spectrometer installed in DuMond geometry. An instrumental resolution of about 10 eV was achieved for Lγ (L-N,O) X-ray transitions, allowing clear separation of M-shell X-ray satellites for Th and U. Moreover, the N-shell satellite structure in the Lγ6 (L2-O4) X-ray transition was observed for 360-MeV O ion impact on a thorium target. This, to our knowledge, is the first observation of this kind. Other observed Lγ X-ray diagram lines are shifted and widened, with respect to the photoinduced X-ray spectra excited by an X-ray tube, due to the unresolved N-shell and, probable the O-shell, satellite structure.

We propose a novel approach for the theoretical analysis of the photoinduced high-resolution K(h)α(1,2) x-ray hypersatellite spectra, which allows us to obtain reliable values of lifetimes of the doubly K-shell ionized states and fundamental information about the relative role of K-shell double photoionization (DPI) mechanisms. It is demonstrated for the first time that the K(h)α(1,2) hypersatellite natural line broadening observed for selected metal atoms with 20 ≤ Z ≤ 30 can be well reproduced quantitatively by taking into account the influences of the open-shell valence configuration (adopted from predictions of the band-structure method) and the outer-shell ionization and excitation following the DPI process.

Single-photon double $K$-shell ionization of low-$Z$ neutral atoms in the range $12\ensuremath{\leqslant}Z\ensuremath{\leqslant}23$ is investigated. The experimental method was based on measurements of the high-resolution $K\ensuremath{\alpha}{}^{h}$ hypersatellite x-ray spectra following the radiative decay of the $K$-shell double-vacancy states excited by monochromatic synchrotron radiation. The photon energy dependence of the double $K$-shell ionization was measured over a wide range of photon energies from threshold up to and beyond the maximum of the double-to-single photoionization cross section ratios. From the high-resolution x-ray emission spectra the energies and linewidths of the hypersatellite transitions, as well as the $K{\ensuremath{\alpha}}_{1}^{h}$:$K{\ensuremath{\alpha}}_{2}^{h}$ intensity ratios, were determined. The relative importance of the initial-state and final-state electron-electron interactions to the $K$-shell double photoionization is addressed. Physical mechanisms and scaling laws of the $K$-shell double photoionization are examined. A semiempirical universal scaling of the double-photoionization cross sections with the effective nuclear charge for neutral atoms in the range $2\ensuremath{\leqslant}Z\ensuremath{\leqslant}47$ is established.

An observation of the internal structure of the L-shell hypersatellite x rays resulting from the one-photon decay of L{sup -2} double-vacancy states in palladium multiply ionized by oxygen ions is reported. The Pd L{sub 3}{yields}M{sub 4,5} x-ray spectrum was measured with a von Hamos high-resolution crystal spectrometer. The complex shape of the observed spectrum could be interpreted in detail using relativistic multiconfiguration Dirac-Fock calculations. The relative intensities of the measured x rays were found to be in good agreement with semiclassical approximation calculations using relativistic Dirac-Hartree-Fock wave functions.

The multiple ionization of the L- and M-shells of Pd by fast oxygen ions has been studied by measuring with high-resolution the satellite structures of the Lα1,2 X-ray transitions. Relativistic multi-configuration Dirac-Fock (MCDF) calculations were used to interpret the complex X-ray spectrum, allowing to derive the number of L- and M-shell spectator vacancies at the moment of the X-ray emission. After correcting these numbers for the atomic vacancy rearrangement processes that take place prior to the X-ray emission, the ionization probabilities corresponding to the collision time were obtained. The latter were compared to predictions of the semiclassical approximation (SCA) and the geometrical model. The SCA calculations were performed using relativistic hydrogenic and self-consistent Dirac-Hartree-Fock (DHF) electronic wave functions. It was found that the use of the more realistic DHF wave functions in the SCA calculations leads to a much better description of the measured ionization probabilities for both the L- and M-shells.

The xenon $L$-subshell Coster-Kronig (CK) transition yields were revisited via high-resolution measurements of the $L{\ensuremath{\alpha}}_{1,2}$ (${L}_{3}\ensuremath{-}{M}_{4,5}$) and $L{\ensuremath{\beta}}_{1}$ (${L}_{2}\ensuremath{-}{M}_{4}$) x-ray emission lines. The $L$ x-ray spectra were measured employing a Johansson-type curved crystal spectrometer and energy-tunable synchrotron radiation. The CK yields were derived from the relative $L$ x-ray intensity jumps at the $L$ edges by fitting the fluorescence intensities as a function of the photon energy to the $L$-subshell photoionization cross sections. The latter were obtained from the measured $L$-edge photoabsorption spectrum. Values of $0.118\ifmmode\pm\else\textpm\fi{}0.029$, $0.383\ifmmode\pm\else\textpm\fi{}0.037$, and $0.096\ifmmode\pm\else\textpm\fi{}0.016$ were found for the ${f}_{23}$, ${f}_{13}$, and ${f}_{12}$ CK yields, respectively. Thanks to high resolution, the ${L}_{1}$ fluorescence yield of $0.059\ifmmode\pm\else\textpm\fi{}0.002$ was also determined from intensity ratios of the well-resolved $L{\ensuremath{\beta}}_{4}$ (${L}_{1}\ensuremath{-}{M}_{2}$) and $L{\ensuremath{\beta}}_{1}$ (${L}_{2}\ensuremath{-}{M}_{4}$) lines.

The K\ensuremath{\alpha} and K\ensuremath{\beta} x-ray spectra of molybdenum bombarded by 5.5-MeV/amu $^{16}\mathrm{O}$ ions were measured with high resolution. In such heavy-ion--atom collisions, multiple ionization of the M and L shells of the target atoms is extremely likely to occur, resulting in a complex structure of the observed spectra. The ${\mathit{L}}^{\mathit{n}}$-satellite structure was resolved, whereas M vacancies produce only a shift and a broadening of the lines so that it is not possible to obtain in a direct way information about the M-hole distribution. We thus propose a method for the analysis of x-ray spectra of multiply ionized atoms. In this method the measured K\ensuremath{\alpha} and K\ensuremath{\beta} spectra are simultaneously analyzed as a sum of K\ensuremath{\alpha}${\mathit{L}}^{\mathit{n}}$${\mathit{M}}^{\mathit{m}}$ and K\ensuremath{\beta}${\mathit{L}}^{\mathit{n}}$${\mathit{M}}^{\mathit{m}}$ components, respectively, with theoretically determined profiles. A binomial distribution of holes in the M shell is assumed and the M-shell ionization probabilities are treated as adjustable parameters. The profiles are constructed as sums of Voigt functions, whose positions and heights are determined by extensive multiconfiguration Dirac-Fock method calculations. If, in a simultaneous fit to the K\ensuremath{\alpha}${\mathit{L}}^{0}$ and K${\mathrm{\ensuremath{\beta}}}_{1,3}$${\mathit{L}}^{0}$ lines, just one parameter ${\mathit{p}}_{\mathit{M}}^{\mathit{X}}$ describing the M-shell ionization at the moment of the K x-ray transition is used, the experimental data are not reproduced in an entirely satisfactory way (${\mathit{p}}_{\mathit{M}}^{\mathit{X}}$=0.19\ifmmode\pm\else\textpm\fi{}0.02). Therefore, two parameters, one common for the 3s and 3p subshells ${\mathit{p}}_{3\mathit{s}\mathit{p}}^{\mathit{X}}$ and the other for the 3d subshells, were introduced and a much better fit to both lines (${\mathit{p}}_{3\mathit{s}\mathit{p}}^{\mathit{X}}$=0.17\ifmmode\pm\else\textpm\fi{}0.02, ${\mathit{p}}_{3\mathit{d}}^{\mathit{X}}$=0.23\ifmmode\pm\else\textpm\fi{}0.02) was obtained.The importance and influence of alternative ionizing processes as electron-capture and rearrangement processes are discussed and the M-shell ionization probability at the moment of the collision (${\mathit{p}}_{\mathit{M}}$=0.18\ifmmode\pm\else\textpm\fi{}0.02) is deduced from the ${\mathit{p}}_{\mathit{M}}^{\mathit{X}}$ value. It is shown that the differences between ${\mathit{p}}_{3\mathit{s}\mathit{p}}^{\mathit{X}}$ and ${\mathit{p}}_{3\mathit{d}}^{\mathit{X}}$ are mainly due to Coster-Kronig transitions, rather than due to different subshell ionization probabilities. The spectra were also analyzed with respect to the L-shell ionization on the basis of the calculated K\ensuremath{\alpha}${\mathit{L}}^{\mathit{n}}$${\mathit{M}}^{0}$, K${\mathrm{\ensuremath{\beta}}}_{1,3}$${\mathit{L}}^{\mathit{n}}$${\mathit{M}}^{0}$, and K${\mathrm{\ensuremath{\beta}}}_{2}$${\mathit{L}}^{\mathit{n}}$${\mathit{M}}^{0}$ components. The M-shell ionization was taken into account by taking a larger Gaussian width and by shifting the positions of the lines. The intensity yields of the L satellites were determined, the primary vacancy distribution was deduced, and the results from K\ensuremath{\alpha} and K\ensuremath{\beta} spectra are compared.