Quantized form factor shift in the presence of free electron laser radiation

In electron scattering, the target form factors contribute significantly to the diffraction pattern and carry information on the target electromagnetic charge distribution. Here we show that the presence of electromagnetic radiation, as intense as currently available in Free Electron Lasers, shifts the dependence of the target form factors by a quantity that depends on the number of photons absorbed or emitted by the electron as well as on the parameters of the electromagnetic radiation. As example, we show the impact of intense ultraviolet and soft X-ray radiation on elastic electron scattering by Ne-like Argon ion and by Xenon atom. We find that the shift brought by the radiation to the form factor is in the order of some percent. Our results may open up a new avenue to explore matter with the assistance of laser

Analytical evaluation of atomic form factors: application to Rayleigh scattering

Atomic form factors are widely used for the characterization of targets and specimens, from crystallography to biology. By using recent mathematical results, here we derive an analytical expression for the atomic form factor within the independent particle model constructed from nonrelativistic screened hydrogenic wavefunctions. The range of validity of this analytical expression is checked by comparing the analytically obtained form factors with the ones obtained within the Hartee-Fock method. As an example, we apply our analytical expression for the atomic form factor to evaluate the differential cross section for Rayleigh scattering off neutral atoms.Comment: 7 pages, 1 figur

4d-inner-shell ionization of Xe+ ions and subsequent Auger decay

We have studied Xe+4d inner-shell photoionization in a direct experiment on Xe+ ions, merging an ion and a photon beam and detecting the ejected electrons with a cylindrical mirror analyzer. The measured 4d photoelectron spectrum is compared to the 4d core valence double ionization spectrum of the neutral Xe atom, obtained with a magnetic bottle spectrometer. This multicoincidence experiment gives access to the spectroscopy of the individual Xe2+4d−15p−1 states and to their respective Auger decays, which are found to present a strong selectivity. The experimental results are interpreted with the help of ab initio calculations.1\. Auflag

Auger resonant-Raman decay after Xe L-edge photoexcitation

We have investigated resonant Auger decay of xenon following photoexcitation of each of the three L edges under resonant-Raman conditions, which allowed us to characterize several higher Rydberg transitions. Relative intensities for spectator final states reached after L1−, L2−, and L3-edge excitations are studied in detail. Thanks to state-of-the-art experimental arrangements, our results not only reproduce the previously calculated 3d−25d and nd(n>5) state cross sections after L3 excitation, but also allow extracting the 3d−26d spectator state energy position and revealing its resonant behavior, blurred by the insufficient experimental resolution in previous data sets. The 3d−26p and 3d−27p states reached after L1 excitation as well as the 3d−25d and 3d−26d states reached after L2 excitation are also investigated and their relative intensities are reported and compared to ab initio Dirac-Hartree-Fock configuration-interaction calculations. We found the signature of electronic- state-lifetime interference effects between several coherently excited intermediate states, due to large lifetime broadening. Electron recapture processes are also identified above all three photoionization thresholds

Deep-core photoionization of krypton atoms below and above the 1s ionization threshold

Electronic relaxation of atomic Kr below and above the 1s ionization threshold is investigated experimentally using hard x-ray photoelectron spectroscopy. The experimental results are interpreted with the aid of relativistic Dirac-Fock calculations. The 1s orbital core-hole lifetime is extracted and the satellite's structures accompanying the photoelectron main line are assigned. Auger spectra recorded below and above the K edge are also investigated. In particular, the Auger cascade originating from vacancies of different origin in the L shell is analyzed in great detail. Competition between radiative KL versus nonradiative KLL Auger emission is emphasized

Selecting core-hole localization or delocalization in CS2 by photofragmentation dynamics.

Electronic core levels in molecules are highly localized around one atomic site. However, in single-photon ionization of symmetric molecules, the question of core-hole localization versus delocalization over two equivalent atoms has long been debated as the answer lies at the heart of quantum mechanics. Here, using a joint experimental and theoretical study of core-ionized carbon disulfide (CS2), we demonstrate that it is possible to experimentally select distinct molecular-fragmentation pathways in which the core hole can be considered as either localized on one sulfur atom or delocalized between two indistinguishable sulfur atoms. This feat is accomplished by measuring photoelectron angular distributions within the frame of the molecule, directly probing entanglement or disentanglement of quantum pathways as a function of how the molecule dissociates

Dynamic screening of a localized hole during photoemission from a metal cluster

Recent advances in attosecond spectroscopy techniques have fueled the interest in the theoretical description of electronic processes taking place in the subfemtosecond time scale. Here we study the coupled dynamic screening of a localized hole and a photoelectron emitted from a metal cluster using a semi-classical model. Electron density dynamics in the cluster is calculated with Time-Dependent Density Functional Theory and the motion of the photoemitted electron is described classically. We show that the dynamic screening of the hole by the cluster electrons affects the motion of the photoemitted electron. At the very beginning of its trajectory, the photoemitted electron interacts with the cluster electrons that pile up to screen the hole. Within our model, this gives rise to a significant reduction of the energy lost by the photoelectron. Thus, this is a velocity dependent effect that should be accounted for when calculating the average losses suffered by photoemitted electrons in metals.Comment: 15 pages, 5 figure

Detailed assignment of normal and resonant Auger spectra of Xe near the L edges

We present a comprehensive experimental and theoretical investigation on the LMM, LMN, and LNN normal Auger spectra of xenon, which reveal excellent agreement with theory when core-hole lifetimes of the two-hole final states are taken into account. Generally, the spectra turned out to be highly complex due to a strong overlap of the Auger transitions subsequent to 2s−11/2, 2p−11/2, and 2p−13/2 ionization. This overlap is due to the splitting of the three initial L core holes and the different final M and N core holes being on the same order of magnitude of several hundred eV. The Auger transitions are assigned in detail based on the theoretical results. Most of the MM, MN, and NN final states are described well based on jj coupling. In addition, we present a detailed assignment of the resonant LM45M45 Auger transition subsequent to the 2s→6p, 7p and 2p→5d, 6d excitations

Potential Energy Surface Reconstruction and Lifetime Determination of Molecular Double-Core-Hole States in the Hard X-Ray Regime

A combination of resonant inelastic x-ray scattering and resonant Auger spectroscopy provides complementary information on the dynamic response of resonantly excited molecules. This is exemplified for CH3I, for which we reconstruct the potential energy surface of the dissociative I 3d−2 double- core-hole state and determine its lifetime. The proposed method holds a strong potential for monitoring the hard x-ray induced electron and nuclear dynamic response of core-excited molecules containing heavy elements, where ab initio calculations of potential energy surfaces and lifetimes remain challenging