| 1. |
- Jahnke, T., et al.
(författare)
-
Inner-Shell-Ionization-Induced Femtosecond Structural Dynamics of Water Molecules Imaged at an X-Ray Free-Electron Laser
- 2021
-
Ingår i: Physical Review X. - : American Physical Society. - 2160-3308. ; 11:4
-
Tidskriftsartikel (refereegranskat)abstract
- The ultrafast structural dynamics of water following inner-shell ionization is a crucial issue in high-energy radiation chemistry. We have exposed isolated water molecules to a short x-ray pulse from a free-electron laser and detected momenta of all produced ions in coincidence. By combining experimental results and theoretical modeling, we can image dissociation dynamics of individual molecules in unprecedented detail. We reveal significant molecular structural dynamics in H2O2+, such as asymmetric deformation and bond-angle opening, leading to two-body or three-body fragmentation on a timescale of a few femtoseconds. We thus reconstruct several snapshots of structural dynamics at different time intervals, which highlight dynamical patterns that are relevant as initiating steps of subsequent radiation-damage processes.
|
|
| 2. |
- Guillemin, R., et al.
(författare)
-
Isotope effects in dynamics of water isotopologues induced by core ionization at an x-ray free-electron laser
- 2023
-
Ingår i: STRUCTURAL DYNAMICS-US. - 2329-7778. ; 10:5
-
Tidskriftsartikel (refereegranskat)abstract
- Dynamical response of water exposed to x-rays is of utmost importance in a wealth of science areas. We exposed isolated water isotopologues to short x-ray pulses from a free-electron laser and detected momenta of all produced ions in coincidence. By combining experimental results and theoretical modeling, we identify significant structural dynamics with characteristic isotope effects in H2O2+, D2O2+, and HDO2+, such as asymmetric bond elongation and bond-angle opening, leading to two-body or three-body fragmentation on a timescale of a few femtoseconds. A method to disentangle the sequences of events taking place upon the consecutive absorption of two x-ray photons is described. The obtained deep look into structural properties and dynamics of dissociating water isotopologues provides essential insights into the underlying mechanisms.
|
|
| 3. |
- Kosugi, S., et al.
(författare)
-
Strong configuration interaction in the 3p photoelectron spectrum of Kr
- 2020
-
Ingår i: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - 2469-9926 .- 2469-9934. ; 101:4
-
Tidskriftsartikel (refereegranskat)abstract
- We measured the Kr photoelectron spectrum in the region close to the 3p ionization threshold. Our high-resolution measurements allowed a clear observation of spectral structures due to electron correlation effects. Analysis based on relativistic multiconfiguration calculations could explain these observed peaks as due to strong configuration interactions between the 3p(-1) state and 3d(-2) nl states. Calculated and experimental data for peak assignments and intensity distributions are in good agreement. In addition, we measured the anisotropy parameter beta, which also agreed well with theory. These findings provide a detailed view of strong configuration interactions between the 3(-1) and 3d(-2)nl inner-shell hole states.
|
|
| 4. |
- Guillemin, R., et al.
(författare)
-
Concerted and sequential three-body fragmentation of deep-core-ionized carbon disulfide
- 2022
-
Ingår i: Physical Chemistry, Chemical Physics - PCCP. - : Royal Society of Chemistry. - 1463-9076 .- 1463-9084. ; 25:1, s. 183-191
-
Tidskriftsartikel (refereegranskat)abstract
- Momentum vector correlation is a powerful tool to study molecular dissociation. We have studied the three-body fragmentation of carbon disulfide after sulfur 1s photoionization by means of momentum imaging techniques. Concerted and sequential pathways are disentangled in three-body fragmentation using adapted analysis strategies. In particular, we introduce various data visualization schemes that are proved to be particularly efficient to determine dissociation dynamics.
|
|
| 5. |
- Püttner, R., et al.
(författare)
-
Nonstatistical behavior of the photoionization of spin-orbit doublets
- 2021
-
Ingår i: Journal of Physics B: Atomic, Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 54:8
-
Tidskriftsartikel (refereegranskat)abstract
- The photoionization branching ratios of spin-orbit doublets are studied both experimentally and theoretically at energies several keV above threshold. The results show significant relativistic effects for Ar 2p in the autoionizing region below the 1s threshold, and large many-body effects for Xe 3d and 4d in the vicinity of the L-shell thresholds. The branching ratios in Xe are also found to vary significantly over very broad multi-keV energy regions both above and below the inner-shell thresholds. In addition, the Ar 2p study confirms experimentally the decades-old theoretical prediction that the nonresonant branching ratio does not approach the statistical (nonrelativistic) value, and, in fact, progressively diverges from statistical with increasing photon energy. © 2021 The Author(s). Published by IOP Publishing Ltd.
|
|
| 6. |
- Travnikova, O., et al.
(författare)
-
Energy dependent relative cross sections in carbon 1s photoionization
- 2020
-
Ingår i: 31ST INTERNATIONAL CONFERENCE ON PHOTONIC, ELECTRONIC AND ATOMIC COLLISIONS (ICPEAC XXXI). - : IOP PUBLISHING LTD.
-
Konferensbidrag (refereegranskat)abstract
- We demonstrate that the possibility of monitoring relative photoionization cross sections over a large photon energy range extending to hard x-rays allows studying and disentangling shake processes and intramolecular inelastic scattering effects. An "EXAFS"-type of oscillatory behaviour of the relative C is cross sections is observed in a wide photon energy range up to 1 keV due to multiple intramolecular elastic scattering of the photoelectron. These effects are also present in solids and constitute a significant part of all elastic and inelastic scattering effects occurring in solids.
|
|
| 7. |
- Travnikova, O., et al.
(författare)
-
Photochemical Ring-Opening Reaction of 1,3-Cyclohexadiene: the True Reactive State
- 2022
-
Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 144:48, s. 21878-21886
-
Tidskriftsartikel (refereegranskat)abstract
- The photochemically induced ring-opening isomeriza-tion reaction of 1,3-cyclohexadiene to 1,3,5-hexatriene is a textbook example of a pericyclic reaction and has been amply investigated with advanced spectroscopic techniques. The main open question has been the identification of the single reactive state which drives the process. The generally accepted description of the isomerization pathway starts with a valence excitation to the lowest lying bright state, followed by a passage through a conical intersection to the lowest lying doubly excited state, and finally a branching between either the return to the ground state of the cyclic molecule or the actual ring-opening reaction leading to the open-chain isomer. Here, in a joint experimental and computational effort, we demonstrate that the evolution of the excitation-deexcitation process is much more complex than that usually described. In particular, we show that an initially high-lying electronic state smoothly decreasing in energy along the reaction path plays a key role in the ring-opening reaction.
|
|
| 8. |
- Boudjemia, N., et al.
(författare)
-
Electron spectroscopy and dynamics of HBr around the Br 1s(-1) threshold
- 2020
-
Ingår i: Physical Chemistry Chemical Physics. - : Royal Society of Chemistry (RSC). - 1463-9076 .- 1463-9084. ; 22:46, s. 26806-26818
-
Tidskriftsartikel (refereegranskat)abstract
- A comprehensive electron spectroscopic study combined with partial electron yield measurements around the Br 1s ionization threshold of HBr at approximately equal to 13.482 keV is reported. In detail, the Br 1s(-1) X-ray absorption spectrum, the 1s(-1) photoelectron spectrum as well as the normal and resonant KLL Auger spectra are presented. Moreover, the L-shell Auger spectra measured with photon energies below and above the Br 1s(-1) ionization energy as well as on top of the Br 1s(-1)sigma* resonance are shown. The latter two Auger spectra represent the second step of the decay cascade subsequent to producing a Br 1s(-1) core hole. The measurements provide information on the electron and nuclear dynamics of deep core-excited states of HBr on the femtosecond timescale. From the different spectra the lifetime broadening of the Br 1s(-1) single core-hole state as well as of the Br(2s(-2),2s(-1)2p(-1),2p(-2)) double core-hole states are extracted and discussed. The slope of the strongly dissociative HBr 2p(-2)sigma* potential energy curve is found to be about -13.60 eV angstrom(-1). The interpretation of the experimental data, and in particular the assignment of the spectral features in the KLL and L-shell Auger spectra, is supported by relativistic calculations for HBr molecule and atomic Br.
|
|
| 9. |
- Goldsztejn, G., et al.
(författare)
-
Simulation of Auger decay dynamics in the hard X-ray regime : HCl as a showcase
- 2022
-
Ingår i: Physical Chemistry, Chemical Physics - PCCP. - : Royal Society of Chemistry. - 1463-9076 .- 1463-9084. ; 24:11, s. 6590-6604
-
Tidskriftsartikel (refereegranskat)abstract
- Auger decay after photoexcitation or photoemission of an electron from a deep inner shell in the hard X-ray regime can be rather complex, implying a multitude of phenomena such as multiple-step cascades, post-collision interaction (PCI), and electronic state-lifetime interference. Furthermore, in a molecule nuclear motion can also be triggered. Here we discuss a comprehensive theoretical method which allows us to analyze in great detail Auger spectra measured around an inner-shell ionization threshold. HCl photoexcited or photoionized around the deep Cl 1s threshold is chosen as a showcase. Our method allows calculating Auger cross sections considering the nature of the ground, intermediate and final states (bound or dissociative), and the evolution of the relaxation process, including both electron and nuclear dynamics. In particular, we show that we can understand and reproduce a so-called experimental 2D-map, consisting of a series of resonant Auger spectra measured at different photon energies, therefore obtaining a detailed picture of all above-mentioned dynamical phenomena at once.
|
|
| 10. |
- Kosugi, S., et al.
(författare)
-
Conjugate photoelectron recapture peaks in the high resolution Auger electron spectra following near-threshold Ar 2p photoionization
- 2020
-
Ingår i: Journal of Physics B. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 53:12
-
Tidskriftsartikel (refereegranskat)abstract
- We have observed formation of Rydberg series superimposed on the Ar (L3M2,3M2,3) Auger electron spectral profile with photoexcitation just above the 2p(3/2)(-1) photoionization threshold. This is due to the recapture of photoelectrons induced by post-collision interaction between the Auger electron and photoelectron: Ar+ 2p(3/2)(-1) + e(-) -> Ar+ 3p(-2)ml + e(-). The intensity distribution of the angular momentum state resolved Rydberg peaks revealed prominent conjugate peaks due to angular momentum exchange between photoelectrons and Auger electrons in the process. In addition, we measured the 2p(3/2)(-1)nl -> 3p(-2)ml + e(-) resonant Auger spectra with high resolution below the 2p(3/2)(-1) threshold. Our results showed that conjugate shake-up/down 2p(3/2)(-1)nd -> 3p(-2)mp + e(-) processes are stronger than the direct 2p(3/2)(-1)nd -> 3p(-2)ms, (m-1)d + e(-) processes in the spectator Auger processes, implying a strong angular momentum exchange effect between photoelectron and Auger electron.
|
|
