| 1. |
- Jahnke, T., et al.
(författare)
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Inner-Shell-Ionization-Induced Femtosecond Structural Dynamics of Water Molecules Imaged at an X-Ray Free-Electron Laser
- 2021
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Ingår i: Physical Review X. - : American Physical Society. - 2160-3308. ; 11:4
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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.
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| 2. |
- Düsterer, S., et al.
(författare)
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Angle resolved photoelectron spectroscopy of two-color XUV-NIR ionization with polarization control
- 2016
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Ingår i: Journal of Physics B: Atomic, Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 49:16
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Tidskriftsartikel (refereegranskat)abstract
- Electron emission caused by extreme ultraviolet (XUV) radiation in the presence of a strong near infrared (NIR) field leads to multiphoton interactions that depend on several parameters. Here, a comprehensive study of the influence of the angle between the polarization directions of the NIR and XUV fields on the two-color angle-resolved photoelectron spectra of He and Ne is presented. The resulting photoelectron angular distribution strongly depends on the orientation of the NIR polarization plane with respect to that of the XUV field. The prevailing influence of the intense NIR field over the angular emission characteristics for He(1s) and Ne(2p) ionization lines is shown. The underlying processes are modeled in the frame of the strong field approximation (SFA) which shows very consistent agreement with the experiment reaffirming the power of the SFA for multicolor-multiphoton ionization in this regime.
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| 3. |
- Ueda, K, et al.
(författare)
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Nuclear motion and symmetry breaking of the B 1s-excited BF3 molecule
- 2003
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Ingår i: Chemical Physics. - 0301-0104. ; 289:1, s. 135-147
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Tidskriftsartikel (refereegranskat)abstract
- Out-of-plane nuclear motion stimulated in the core-excited state and symmetry breaking due to this nuclear motion have been investigated for B Is excitation in the BF3 molecule by a combination of three different experimental methods: angle-resolved ion-yield spectroscopy, vibrationally resolved resonant Auger electron spectroscopy and quadruple-ion coincidence momentum-imaging technique. (C) 2002 Elsevier Science B.V. All rights reserved.
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| 4. |
- Baev, A., et al.
(författare)
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Doppler interference in dissociative resonant photoemission
- 2002
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Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 66:2
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Tidskriftsartikel (refereegranskat)abstract
- Resonant photoemission involving dissociative core excited states has been the subject of a great number of experimental and theoretical investigations in recent time. The resonant decay of such dissociating systems has been shown to lead to semiatomic Auger electron emission spectra, with particular angular behavior. In the present paper a detailed theoretical analysis of dissociative resonant photoemission spectra of homonuclear diatomic molecules is presented. The theory addresses both fixed in space and randomly oriented homonuclear molecules and emphasizes the Doppler effect and the role of the interference between channels referring to the Doppler split atomic fragments. It is shown that peaks originating from decay in the atomic fragments can be asymmetric and structured due to the Doppler interference effect. The predicted strong non-Lorentzian behavior of the substructure on the top of the Doppler broadened atomiclike contribution is traced to the interplay between decay channels leading to gerade and ungerade final states. Simulations based on wave-packet theory are compared with experimental data for molecular oxygen. Our numerical simulations of the atomiclike resonance of fixed in space molecules show that the spectral profile is very sensitive to the shape of interatomic potentials of core excited and final states. It is shown that the Doppler effect in the decay spectra depends upon the symmetry of the core excited state.
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| 5. |
- Düsterer, S, et al.
(författare)
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Two-color XUV+NIR femtosecond photoionization of neon in the near-threshold region
- 2019
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Ingår i: New Journal of Physics. - : IOP Publishing. - 1367-2630. ; 21
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Tidskriftsartikel (refereegranskat)abstract
- Results of angle-resolved electron spectroscopy of near-threshold photoionization of Ne atoms by combined femtosecond extreme ultraviolet and near infrared fields are presented. The dressed-electron spectra show an energetic distribution into so-called sidebands, being separated by the photon energy of the dressing laser. Surprisingly, for the low kinetic energy (few eV) sidebands, the photoelectron energy varies as a function of the emission angle. Such behavior has not yet been observed in sideband creation and has not been predicted in commonly used theoretical descriptions such as strong field approximation and soft photon approach. Describing the photoionization with a time-dependent Schrödinger equation allows a qualitative description of the observed effect, as well as the prediction of fine structure in the sideband distribution.
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| 6. |
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| 7. |
- Ilchen, M., et al.
(författare)
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X-ray spectroscopy on ultrafast-decaying core-excited atomic ions
- 2020
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Ingår i: Charge-exchange. - : IOP Publishing. - 1742-6588. ; 1412
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Konferensbidrag (refereegranskat)abstract
- Results from the first soft X-ray user experiment at the European XFEL on nonlinear photon-matter interaction will be presented. Angle-resolved electron time-of-flight spectroscopy employed at the AQS (Atomic- like Quantum Systems) endstation of the SQS (Small Quantum Systems) instrument reveals insight into the character of resonances in highly transient, core ionized neon ions, i.e. Ne:+ 1s12s22p6 → Ne+&∗ 1s02s22p6np, together with their respective relaxation dynamics. Enabled by the unique properties of the European XFEL, novel perspectives on efficient nonlinear spectroscopy will be discussed.
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| 8. |
- Kitajima, M., et al.
(författare)
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Doppler effect in resonant photoemission from SF6 : Correlation between doppler profile and auger emission anisotropy
- 2003
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Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 91:21
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Tidskriftsartikel (refereegranskat)abstract
- Fragmentation of the SF6 molecule upon F 1s excitation has been studied by resonant photoemission. The F atomiclike Auger line exhibits the characteristic Doppler profile that depends on the direction of the photoelectron momentum relative to the polarization vector of the radiation as well as on the photon energy. The measured Doppler profiles are analyzed by the model simulation that takes account of the anisotropy of the Auger emission in the molecular frame. The Auger anisotropy extracted from the data decreases with an increase in the F-SF5 internuclear distance.
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| 9. |
- Mazza, T., et al.
(författare)
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Mapping Resonance Structures in Transient Core-Ionized Atoms
- 2020
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Ingår i: Physical Review X. - 2160-3308. ; 10:4
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Tidskriftsartikel (refereegranskat)abstract
- The nature of transient electronic states created by photoabsorption critically determines the dynamics of the subsequently evolving system. Here, we investigate K-shell photoionized atomic neon by absorbing a second photon within the Auger-decay lifetime of 2.4 fs using the European XFEL, a unique high-repetition-rate, wavelength-tunable x-ray free-electron laser. By high-resolution electron spectroscopy, we map out the transient Rydberg resonances unraveling the details of the subsequent decay of the hollow atom. So far, ultra-short-lived electronic transients, which are often inaccessible by experiments, were mainly inferred from theory but are now addressed by nonlinear x-ray absorption. The successful characterization of these resonances with femtosecond lifetimes provides the basis for a novel class of site-specific, nonlinear, and time-resolved studies with strong impact for a wide range of topics in physics and chemistry.
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| 10. |
- Travnikova, O., et al.
(författare)
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Photochemical Ring-Opening Reaction of 1,3-Cyclohexadiene: the True Reactive State
- 2022
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Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 144:48, s. 21878-21886
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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.
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| 11. |
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| 12. |
- Eichmann, U., et al.
(författare)
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Photon-recoil imaging : Expanding the view of nonlinear x-ray physics
- 2020
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Ingår i: Science. - : AMER ASSOC ADVANCEMENT SCIENCE. - 0036-8075 .- 1095-9203. ; 369:6511, s. 1630-1633
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Tidskriftsartikel (refereegranskat)abstract
- Addressing the ultrafast coherent evolution of electronic wave functions has long been a goal of nonlinear x-ray physics. A first step toward this goal is the investigation of stimulated x-ray Raman scattering (SXRS) using intense pulses from an x-ray free-electron laser. Earlier SXRS experiments relied on signal amplification during pulse propagation through dense resonant media. By contrast, our method reveals the fundamental process in which photons from the primary radiation source directly interact with a single atom. We introduce an experimental protocol in which scattered neutral atoms rather than scattered photons are detected. We present SXRS measurements at the neon K edge and a quantitative theoretical analysis. The method should become a powerful tool in the exploration of nonlinear x-ray physics.
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| 13. |
- Feifel, R, et al.
(författare)
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Probing doubly excited ionic states of N-2(+) via a triple excitation above the N 1s threshold in the N-2 molecule
- 2003
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Ingår i: Physical Review A (Atomic, Molecular and Optical Physics). - 1050-2947. ; 67:3: 032504
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Tidskriftsartikel (refereegranskat)abstract
- Angle-resolved resonant Auger-electron spectroscopy has been carried out on the nitrogen molecule at selected photon energies around 419 eV, where a 1s core electron and two valence electrons are promoted into the lowest unoccupied molecular orbital 1pi(g). Significant enhancement of a specific band, which cannot be disentangled in direct photoionization, is observed at a binding energy of 37.6 eV, with a value of the anisotropy parameter beta much smaller than 2. We assign this new band to the transition to a doubly excited cationic state of N-2, in which two of the excited valence electrons remain in the 1pi(g) orbital, proposing a "double spectator" type decay mechanism. This observation shows how to preferentially probe multiply excited configurations of cations using multiple resonant excitation.
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| 14. |
- Feifel, Raimund, et al.
(författare)
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Probing the valence character of O-1s -> Rydberg excited O-2 by participator Auger decay measurements and partial ion yield spectroscopy following x-ray absorption
- 2007
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 126:17, s. 174304-
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Tidskriftsartikel (refereegranskat)abstract
- The valence character of O 1s -> Rydberg excited O-2 is investigated by means of participator Auger decay spectroscopy, performed at selected photon energies across the K-shell resonance region, and by means of partial ion yield x-ray absorption spectroscopy. For several of the excitation energies studied, the authors find substantial sigma(*)((4)Sigma(-)(u),(2)Sigma(-)(u)) valence character being mixed with ns sigma and np sigma ((4)Sigma(-)(u),(2)Sigma(-)(u)) Rydberg states. An experimental indication of a coupling between the channels associated with quartet and doublet ion cores is considered and discussed. New spectroscopic constants are derived for the singly ionized X (2)Pi(g) state of O-2 based on the observation of at least 20 vibrational sublevels.
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| 15. |
- Feifel, R., et al.
(författare)
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X-ray absorption and resonant Auger spectroscopy of O(2) in the vicinity of the O 1s ->sigma* resonance : Experiment and theory
- 2008
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Ingår i: Journal of Chemical Physics. - : American Institute of Physics (AIP). - 0021-9606 .- 1089-7690. ; 128:6
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Tidskriftsartikel (refereegranskat)abstract
- We report on an experimental and theoretical investigation of x-ray absorption and resonant Auger electron spectra of gas phase O(2) recorded in the vicinity of the O 1s ->sigma* excitation region. Our investigation shows that core excitation takes place in a region with multiple crossings of potential energy curves of the excited states. We find a complete breakdown of the diabatic picture for this part of the x-ray absorption spectrum, which allows us to assign an hitherto unexplained fine structure in this spectral region. The experimental Auger data reveal an extended vibrational progression, for the outermost singly ionized X (2)Pi(g) final state, which exhibits strong changes in spectral shape within a short range of photon energy detuning (0 eV>Omega>-0.7 eV). To explain the experimental resonant Auger electron spectra, we use a mixed adiabatic/diabatic picture selecting crossing points according to the strength of the electronic coupling. Reasonable agreement is found between experiment and theory even though the nonadiabatic couplings are neglected. The resonant Auger electron scattering, which is essentially due to decay from dissociative core-excited states, is accompanied by strong lifetime-vibrational and intermediate electronic state interferences as well as an interference with the direct photoionization channel. The overall agreement between the experimental Auger spectra and the calculated spectra supports the mixed diabatic/adiabatic picture.
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| 16. |
- Feinberg, Alexandra J., et al.
(författare)
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X-ray diffractive imaging of highly ionized helium nanodroplets
- 2022
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Ingår i: Physical Review Research. - 2643-1564. ; 4:2
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Tidskriftsartikel (refereegranskat)abstract
- Finding the lowest energy configuration of N unit charges on a sphere, known as Thomson's problem, is a long-standing query which has only been studied via numerical simulations. We present its physical realization using multiply charged He nanodroplets. The charge positions are determined by x-ray coherent diffractive imaging with Xe as a contrast agent. In neutral droplets, filaments resulting from Xe atoms condensing on quantum vortices are observed. Unique to charged droplets, however, Xe clusters that condense on charges are distributed on the surface in lattice-like structures, introducing He droplets as experimental model systems for the study of Thomson's problem.
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| 17. |
- Kitajima, M., et al.
(författare)
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Angle-resolved photoion yield and resonant Auger spectroscopy for the doubly excited Rydberg states above the C 1s threshold of CO
- 2008
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Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 78:3, s. 033422-
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Tidskriftsartikel (refereegranskat)abstract
- Doubly excited core-hole states of carbon monoxide in the photon energy region of 300-305 eV, i.e., directly above the C 1s ionization threshold, have been studied using both angle-resolved ion-yield and high-resolution resonant Auger spectroscopies. The leading configurations of the most prominent doubly excited Rydberg states are assigned by careful analysis of the ion-yield spectra and the final-state spectra to C 1s(-1) (5 sigma(-1)2 pi S-1=1) 3s sigma (v'=0,1,2), C 1s(-1) (5 sigma(-1)2 pi S-1=0) 3s sigma (v'=0,1,2), and C 1s(-1) (5 sigma(-1)2 pi S-1=1) 4s sigma (v'=0,1), which can only be populated via a conjugate shake-up process. Analysis of the resonant Auger spectra provides an assignment of several two-hole-one-electron (2h-1e) final states.
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| 18. |
- Müller, L., et al.
(författare)
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Note : Soft X-ray transmission polarizer based on ferromagnetic thin films
- 2018
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Ingår i: Review of Scientific Instruments. - : American Institute of Physics Inc.. - 0034-6748 .- 1089-7623. ; 89:3
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Tidskriftsartikel (refereegranskat)abstract
- A transmission polarizer for producing elliptically polarized soft X-ray radiation from linearly polarized light is presented. The setup is intended for use at synchrotron and free-electron laser beamlines that do not directly offer circularly polarized light for, e.g., X-ray magnetic circular dichroism (XMCD) measurements or holographic imaging. Here, we investigate the degree of ellipticity upon transmission of linearly polarized radiation through a cobalt thin film. The experiment was performed at a photon energy resonant to the Co L3-edge, i.e., 778 eV, and the polarization of the transmitted radiation was determined using a polarization analyzer that measures the directional dependence of photo electrons emitted from a gas target. Elliptically polarized radiation can be created at any absorption edge showing the XMCD effect by using the respective magnetic element.
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| 19. |
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| 20. |
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| 21. |
- Piancastelli, MN, et al.
(författare)
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Resonant auger decay of above-threshold core-excited H2O
- 2005
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Ingår i: Physical Review A (Atomic, Molecular and Optical Physics). - 1050-2947. ; 71:1
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Tidskriftsartikel (refereegranskat)abstract
- The decay properties of an above-threshold resonance in core-ionized water, which is difficult to. identify with usual spectroscopic methods, have been analyzed by resonant Auger spectroscopy. The resonance is. shown to correspond to a doubly excited neutral state embedded in the O 1s ionization continuum. The main, result of the experiments is the assessment on the dissociative nature of the intermediate state, with a consequent fragmentation in H neutral plus O*H core excited. This dissociation takes place on the same time scale.. as electron decay, and therefore is categorized as an ultrafast. dissociation process.
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| 22. |
- R. Feifel, K. Ueda, A. De Fanis, K. Okada, S. Tanimoto, T. Furuta, H. Shindo, M. Kitajima, H. Tanaka, O. Björneholm, L. Karlsson, S. Svensson and S. L. Sorensen
(författare)
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Probing doubly excited ionic states of N2+ via a triple excitation above the N1s threshold in the N2 moecule
- 2003
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Ingår i: Phys. Rev.. ; A:67, s. 32504-
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Tidskriftsartikel (refereegranskat)
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| 23. |
- Ristinmaa Sörensen, Stacey, et al.
(författare)
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Application of an atomic relaxation model for the interpretation of O1s to Rydberg excited Auger electron spectra of molecular oxygen
- 2004
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Ingår i: Chemical Physics Letters. - : Elsevier BV. - 0009-2614. ; 398:1-3, s. 168-174
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Tidskriftsartikel (refereegranskat)abstract
- Resonant and normal Auger electron spectra associated with an O1s initial vacancy of the O-2 molecule have been recorded using photon energies of 541.80, 541.97 and 650 eV. The resonant Auger spectra obtained at 541.80 and 541.97 eV are interpreted as composed essentially of two characteristic parts, one between 10 and 35 eV binding energy reminiscent to direct photoionisation, and another, above 35 eV, associated primarily with spectator decay of the intermediate core-hole state. The spectra above 35 eV owe some similarity to the ordinary Auger electron spectrum recorded at 650 eV, and an interpretation is made in terms of Rydberg series in the cation converging towards the dicationic ionisation limits. The interpretation is based on a relaxation model introduced earlier for atomic resonant Auger spectra. The assignments of the resonant spectra assume that the relevant intermediate neutral states at 541.80 and 541.97 eV governing the Auger decay are essentially the v = 0 and 1 vibrational components of the (O1s) ((4)Sigma(u)(-)) 4psigma Rydberg state. Arguments for this interpretation are given.
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| 24. |
- Sankari, R, et al.
(författare)
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High resolution O 1s photoelectron shake-up satellite spectrum of H2O
- 2006
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Ingår i: Chemical Physics Letters. - : Elsevier BV. - 0009-2614. ; 422:1-3, s. 51-57
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Tidskriftsartikel (refereegranskat)abstract
- The O 1s photoelectron satellite spectrum of water has been recorded with high resolution and some vibrational structures were detected. The electronic and vibrational structures observed in the experimental spectrum are well interpreted with the aid of the molecular ab initio calculations based on the symmetry adapted cluster-configuration interaction (SAC-CI) method. (c) 2006 Elsevier B.V. All rights reserved.
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| 25. |
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