Argon as a showcase

Electronic-state–lifetime interference is a phenomenon specific for ionization of atoms and molecules in the hard-x-ray regime. Using resonant KL2,3L2,3 Auger decay in argon as a showcase, we present a model that allows extracting the interference terms directly from the cross sections of the final electronic states. The analysis provides fundamental information on the excitation and decay processes such as probabilities of various decay paths and the values of the dipole matrix elements for transitions to the excited states. Our results shed light on the interplay between spectator, shake-down, and shake-up processes in the relaxation of deep core-hole states

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

Collinear helium under periodic driving: stabilization of the asymmetric stretch orbit

The collinear eZe configuration of helium, with the electrons on opposite sides of the nucleus, is studied in the presence of an external electromagnetic (laser or microwave) field. We show that the classically unstable "asymmetric stretch" orbit, on which doubly excited intrashell states of helium with maximum interelectronic angle are anchored, can be stabilized by means of a resonant driving where the frequency of the electromagnetic field equals the frequency of Kepler-like oscillations along the orbit. A static magnetic field, oriented parallel to the oscillating electric field of the driving, can be used to enforce the stability of the configuration with respect to deviations from collinearity. Quantum Floquet calculations within a collinear model of the driven two-electron atom reveal the existence of nondispersive wave packets localized on the stabilized asymmetric stretch orbit, for double excitations corresponding to principal quantum numbers of the order of N > 10.Comment: 13 pages, 12 figure

Electronic-state–lifetime interference in the hard-x-ray regime: Argon as a showcase

International audienceElectronic-state–lifetime interference is a phenomenon specific for ionization of atoms and molecules in the hard-x-ray regime. Using resonant KL 2,3 L 2,3 Auger decay in argon as a showcase, we present a model that allows extracting the interference terms directly from the cross sections of the final electronic states. The analysis provides fundamental information on the excitation and decay processes such as probabilities of various decay paths and the values of the dipole matrix elements for transitions to the excited states. Our results shed light on the interplay between spectator, shake-down, and shake-up processes in the relaxation of deep core-hole states

The O K-2V spectrum of CO : the influence of the second core-hole

Using synchrotron radiation in the tender X-ray regime, a photoelectron spectrum showing the formation of single site double-core-hole pre-edge states, involving the K shell of the O atom in CO, has been recorded by means of high-resolution electron spectroscopy. The experimentally observed structures have been simulated, interpreted and assigned, employing state-of-the-art ab initio quantum chemical calculations, on the basis of a theoretical model, accounting for their so-called direct or conjugate character. Features appearing above the double ionization threshold have been reproduced by taking into account the strong mixing between multi-excited and continuum states. The shift of the σ* resonance below the double ionization threshold, in combination with the non-negligible contributions of multi-excited configurations in the final states reached, gives rise to a series of avoided crossings between the different potential energy curves

Interplay of complex decay processes after argon 1s ionization

Abstract Complex decay pathways involving radiative and nonradiative relaxation after deep core-level ionization in argon are disentangled by a unique combination of several synchrotron radiation-based spectroscopic techniques. In particular, by comparing the results obtained from electron-ion coincidence, photon-ion coincidence, and x-ray emission measurements, we are able to distinguish the final ionic states produced in the cascade decay involving Kα and Kβ radiative decay and final ionic states produced by nonradiative cascade decay. High-resolution Auger electron spectroscopy is then used as a complementary tool to identify the LMM transitions contributing to the cascade decay. Ab initio calculations are performed to identify the electronic states involved in the LMM decay