Direct Observation of Double-Core-Hole Shake-Up States in Photoemission

Püttner, R.; Goldsztejn, Gildas; Céolin, Denis; Rueff, Jean‐Pascal; Moreno, Thierry; Kushawaha, Rajesh K.; Marchenko, T.; Guillemin, R.; Journel, L.; Lindle, Dennis W.; Piancastelli, Maria Novella; Simon, M.

doi:10.1103/physrevlett.114.093001

Cited by 41 publications

(77 citation statements)

References 29 publications

(50 reference statements)

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The model threshold energies for 1s + 2s and 1s + 1s double detachment are slightly higher than the calculated threshold energies from Table I for these processes. We attribute this to the fact that the sudden change of the atomic potential following double detachment gives rise to a sizeable shake-up of L-shell electrons as has explicitly been shown, e.g., by Auger electron and photoelectron spectroscopy of double core-hole levels of rare-gas atoms [27][28][29]. The present structure calculations suggest that shake-up processes can shift the double-detachment thresholds of C − to higher energies by up to 20 eV.…”

supporting

confidence: 66%

Multiple Photodetachment of Carbon Anions via Single and Double Core-Hole Creation

Perry‐Sassmannshausen

Buhr

Borovik

et al. 2020

Phys. Rev. Lett.

View full text Add to dashboard Cite

We report on new measurements of m-fold photodetachment (m = 2 − 5) of carbon anions via K-shell excitation and ionization. The experiments were carried out employing the photon-ion merged-beams technique at a synchrotron light source. While previous measurements were restricted to double detachment (m = 2) and to just the lowest-energy K-shell resonance at about 282 eV, our absolute experimental m-fold detachment cross sections at photon energies of up to 1000 eV exhibit a wealth of new thresholds and resonances. We tentatively identify these features with the aid of detailed atomic-structure calculations. In particular, we find unambiguous evidence for fivefold detachment via double K-hole production.Atomic anions are highly correlated systems where the extra electron is weakly bound to an overall neutral charge distribution. Consequently, the number of excited states of atomic anions is quite limited [1] and some atomic species such as nitrogen do not form anions at all. A thorough treatment of the correlation effects in negative atomic ions still poses a formidable challenge to atomic theory, and this becomes even greater for innershell vacancies, since the valence electrons are then subject to strong many-electron relaxation effects following the creation of core holes [2, 3]. On the experimental side, core holes can be readily created by exciting or ionizing an inner-shell electron by a photon. For light ions, the core-hole state will subsequently decay via Auger transitions such that electrons are emitted with the net effect of photoionization. For negative ions, the entire process is termed (multiple) photodetachment.So far, photodetachment via the initial creation of a single K-hole has been experimentally studied only for a limited number of light anions up to F − [3-9]. For C − ions especially, previous measurements were carried out by Gibson et al. [7] and by Walter et al. [8] who studied double photodetachment in a very narrow photon energy range just covering the 1s 2 2s 2 2p 3 4 S → 1s 2s 2 2p 4 4 P resonance at about 282 eV. This scarcity of data is due to the fact that sufficiently high photon fluxes for more comprehensive studies were not available. Here, we present absolute cross sections, σ m , for m-fold photodetachment of C − ions by a single photon,with m = 2, 3, 4, 5 and photon energies from below the K-edge up to ∼1000 eV. These cross sections provide a view of the photodetachment dynamics of a highly correlated atomic system in unprecedented detail. Apart from the resonance at ∼282 eV, we observed a number of additional photodetachment resonances with a variety of line shapes as well as a clear signature for multiple detachment by direct double K-hole production. To better understand these observations, detailed atomic-structure calculations were performed by using the GRASP [10] and RATIP [11] codes as well as the Jena Atomic Calculator (JAC) [12]. To the best of our knowledge, there is only one other theoretical study of highly excited resonances in C − which, however, is focussed exc...

show abstract

supporting

confidence: 66%

Multiple Photodetachment of Carbon Anions via Single and Double Core-Hole Creation

Perry‐Sassmannshausen

Buhr

Borovik

et al. 2020

Phys. Rev. Lett.

View full text Add to dashboard Cite

show abstract

“…the resolving power E/ΔE higher than 5000 (where E is the kinetic energy of electron and ΔE the instrumental resolution), are quite scarce. Up to now, the GALAXIES beamline at the SOLEIL synchrotron [2,3] has been the only facility for high-resolution HAXPES experiments on atomic and molecular science and has been achieving significant results on double-core-hole spectroscopy [4][5][6][7], recoil effects [8][9][10], ultrafast phenomena [11][12][13], post-collision interaction (PCI) [14,15], resonant Auger processes [16][17][18][19][20], and very recent studies on aqueous solution [21,22]. The experiments at the GALAXIES beamline, however, are limited to the excitation energy ranging between 2.3 and 12 keV, while experiments with much higher photon energy are quite scarce.…”

Section: Introductionmentioning

confidence: 99%

Hard x-ray photoelectron spectroscopy on heavy atoms and heavy-element containing molecules using synchrotron radiation up to 35 keV at SPring-8 undulator beamlines

et al. 2019

View full text Add to dashboard Cite

We have recently initiated hard x-ray photoelectron spectroscopy experiments on heavy atoms and heavy-element containing molecules in gas phase by using synchrotron radiation up to 35 keV at SPring-8 undulator beamlines. We have successfully measured deep inner-shell photoelectron spectra, as well as L-MM and M-NN Auger electron spectra excited below and above the K-edge of heavy elements. Target specimens utilized for the preliminary experiments are Ar, Kr and Xe atoms, and also iodine in iodomethane (CH 3 I) and trifluoroiodomethane (CF 3 I) molecules, respectively. We show some selected results on the extracted core-hole lifetime broadenings for the iodine 1s core level of the CH 3 I molecule and also for the Xe 2s, 2p core levels, to compare with theoretical values. The L-MM Auger electron spectra of Kr recorded at 13 and 16.6 keV excitation energies are also shown as typical examples, and the spectrum measured above the K-edge, i.e. 14.327 keV, is analyzed based on theoretical calculations using the Hartree-Fock method. As a result, we give a tentative assignment for the double-core-hole hyper-satellite LL-LMM Auger transitions of the Kr atom.

show abstract

“…Around the same time, Lablanquie and coworkers 6 presented similar studies on N 2 , CO, CO 2 and O 2 . Building on the works of Eland et al 3 and Lablanquie et al, 6 Püttner et al 8 and Goldsztejn et al 9 showed more recently that DCH states of the pre-edge type can also be observed using a high resolution single-channel electron spectroscopy technique for detecting the one core electron which gets ejected into the continuum at a very well defined kinetic energy. With this technique they were able to detect DCH states with binding energies up to 3.5 keV.…”

Section: Introductionmentioning

confidence: 99%

KL double core hole pre-edge states of HCl

Koulentianos

Püttner

Goldsztejn

et al. 2018

Phys. Chem. Chem. Phys.

View full text Add to dashboard Cite

The formation of double core hole pre-edge states of the form 1s2p(P)σ*,nl for HCl, located on the binding energy scale as deep as 3 keV, has been investigated by means of a high resolution single channel electron spectroscopy technique recently developed for the hard X-ray region. A detailed spectroscopic assignment is performed based on ab initio quantum chemical calculations and by using a sophisticated fit model comprising regular Rydberg series. Quantum defects for the different Rydberg series are extracted and the energies for the associated double core hole ionization continua are extrapolated. Dynamical information such as the lifetime width of these double-core-hole pre-edge states and the slope of the related dissociative potential energy curves are also obtained. In addition, 1s2pVnlλn'l'λ' double shake-up transitions and double core hole states of the form 1s2s(S)σ*,4s are observed.

show abstract

Direct Observation of Double-Core-Hole Shake-Up States in Photoemission

Cited by 41 publications

References 29 publications

Multiple Photodetachment of Carbon Anions via Single and Double Core-Hole Creation

Multiple Photodetachment of Carbon Anions via Single and Double Core-Hole Creation

Hard x-ray photoelectron spectroscopy on heavy atoms and heavy-element containing molecules using synchrotron radiation up to 35 keV at SPring-8 undulator beamlines

KL double core hole pre-edge states of HCl

Contact Info

Product

Resources

About