| 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. |
- Guillemin, R., et al.
(författare)
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Isotope effects in dynamics of water isotopologues induced by core ionization at an x-ray free-electron laser
- 2023
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Ingår i: STRUCTURAL DYNAMICS-US. - 2329-7778. ; 10:5
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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.
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| 3. |
- Sanchez-Gonzalez, A., et al.
(författare)
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Accurate prediction of X-ray pulse properties from a free-electron laser using machine learning
- 2017
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 8
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Tidskriftsartikel (refereegranskat)abstract
- Free-electron lasers providing ultra-short high-brightness pulses of X-ray radiation have great potential for a wide impact on science, and are a critical element for unravelling the structural dynamics of matter. To fully harness this potential, we must accurately know the X-ray properties: intensity, spectrum and temporal profile. Owing to the inherent fluctuations in free-electron lasers, this mandates a full characterization of the properties for each and every pulse. While diagnostics of these properties exist, they are often invasive and many cannot operate at a high-repetition rate. Here, we present a technique for circumventing this limitation. Employing a machine learning strategy, we can accurately predict X-ray properties for every shot using only parameters that are easily recorded at high-repetition rate, by training a model on a small set of fully diagnosed pulses. This opens the door to fully realizing the promise of next-generation high-repetition rate X-ray lasers.
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| 4. |
- Allum, F., et al.
(författare)
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A localized view on molecular dissociation via electron-ion partial covariance
- 2022
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Ingår i: Communications Chemistry. - : Springer Science and Business Media LLC. - 2399-3669. ; 5:1
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Tidskriftsartikel (refereegranskat)abstract
- Inner-shell photoelectron spectroscopy provides an element-specific probe of molecular structure, as core-electron binding energies are sensitive to the chemical environment. Short-wavelength femtosecond light sources, such as Free-Electron Lasers (FELs), even enable time-resolved site-specific investigations of molecular photochemistry. Here, we study the ultraviolet photodissociation of the prototypical chiral molecule 1-iodo-2-methylbutane, probed by extreme-ultraviolet (XUV) pulses from the Free-electron LASer in Hamburg (FLASH) through the ultrafast evolution of the iodine 4d binding energy. Methodologically, we employ electron-ion partial covariance imaging as a technique to isolate otherwise elusive features in a two-dimensional photoelectron spectrum arising from different photofragmentation pathways. The experimental and theoretical results for the time-resolved electron spectra of the 4d(3/2) and 4d(5/2) atomic and molecular levels that are disentangled by this method provide a key step towards studying structural and chemical changes from a specific spectator site. Coincidence experiments at free-electron lasers enable time resolved site-specific investigations of molecular photochemistry at high signal rates, but isolating individual dissociation processes still poses a considerable technical challenge. Here, the authors use electron-ion partial covariance imaging to isolate otherwise elusive chemical shifts in UV-induced photofragmentation pathways of the prototypical chiral molecule 1-iodo-2-methylbutane.
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| 5. |
- 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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| 6. |
- Sanchez-Gonzalez, A., et al.
(författare)
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Auger electron and photoabsorption spectra of glycine in the vicinity of the oxygen K-edge measured with an X-FEL
- 2015
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Ingår i: Journal of Physics B-Atomic Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 48:23
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Tidskriftsartikel (refereegranskat)abstract
- We report the first measurement of the near oxygen K-edge auger spectrum of the glycine molecule. Our work employed an x-ray free electron laser as the photon source operated with input photon energies tunable between 527 and 547 eV. Complete electron spectra were recorded at each photon energy in the tuning range, revealing resonant and non-resonant auger structures. Finally ab initio theoretical predictions are compared with the measured above the edge auger spectrum and an assignment of auger decay channels is performed.
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| 7. |
- Hartmann, G., et al.
(författare)
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Circular dichroism measurements at an x-ray free-electron laser with polarization control
- 2016
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Ingår i: Review of Scientific Instruments. - : AIP Publishing. - 0034-6748 .- 1089-7623. ; 87:8
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Tidskriftsartikel (refereegranskat)abstract
- A non-destructive diagnostic method for the characterization of circularly polarized, ultraintense, short wavelength free-electron laser (FEL) light is presented. The recently installed Delta undulator at the LCLS (Linac Coherent Light Source) at SLAC National Accelerator Laboratory (USA) was used as showcase for this diagnostic scheme. By applying a combined two-color, multi-photon experiment with polarization control, the degree of circular polarization of the Delta undulator has been determined. Towards this goal, an oriented electronic state in the continuum was created by non-resonant ionization of the O2 1s core shell with circularly polarized FEL pulses at hν 700 eV. An also circularly polarized, highly intense UV laser pulse with hν 3.1 eV was temporally and spatially overlapped, causing the photoelectrons to redistribute into so-called sidebands that are energetically separated by the photon energy of the UV laser. By determining the circular dichroism of these redistributed electrons using angle resolving electron spectroscopy and modeling the results with the strong-field approximation, this scheme allows to unambiguously determine the absolute degree of circular polarization of any pulsed, ultraintense XUV or X-ray laser source. © 2016 Author(s).
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| 8. |
- Hartmann, N., et al.
(författare)
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Attosecond time-energy structure of X-ray free-electron laser pulses
- 2018
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Ingår i: Nature Photonics. - : Springer Science and Business Media LLC. - 1749-4885 .- 1749-4893. ; 12:4, s. 215-220
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Tidskriftsartikel (refereegranskat)abstract
- The time-energy information of ultrashort X-ray free-electron laser pulses generated by the Linac Coherent Light Source is measured with attosecond resolution via angular streaking of neon 1s photoelectrons. The X-ray pulses promote electrons from the neon core level into an ionization continuum, where they are dressed with the electric field of a circularly polarized infrared laser. This induces characteristic modulations of the resulting photoelectron energy and angular distribution. From these modulations we recover the single-shot attosecond intensity structure and chirp of arbitrary X-ray pulses based on self-amplified spontaneous emission, which have eluded direct measurement so far. We characterize individual attosecond pulses, including their instantaneous frequency, and identify double pulses with well-defined delays and spectral properties, thus paving the way for X-ray pump/X-ray probe attosecond free-electron laser science. © 2018 The Author(s).
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| 9. |
- Heider, R., et al.
(författare)
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Megahertz-compatible angular streaking with few-femtosecond resolution at x-ray free-electron lasers
- 2019
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Ingår i: Physical Review A. - 2469-9926. ; 100:5
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Tidskriftsartikel (refereegranskat)abstract
- Highly brilliant, coherent, femtosecond x-ray pulses delivered by free-electron lasers (FELs) constitute one of the pillars of modern ultrafast science. Next generation FEL facilities provide up to megahertz repetition rates and pulse durations down to the attosecond regime utilizing self-amplification of spontaneous emission. However, the stochastic nature of this generation mechanism demands single-shot pulse characterization to perform meaningful experiments. Here we demonstrate a fast yet robust online analysis technique capable of megahertz-rate mapping of the temporal intensity structure and arrival time of x-ray FEL pulses with few-femtosecond resolution. We performed angular streaking measurements of both neon photo- and Auger electrons and show their applicability for a direct time-domain feedback system during ongoing experiments. The fidelity of the real-time pulse characterization algorithm is corroborated by resolving isolated x-ray pulses and double pulse trains with few-femtosecond substructure, thus paving the way for x-ray-pump-x-ray-probe FEL science at repetition rates compatible with the demands of LCLS-II and European XFEL.
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| 10. |
- 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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| 11. |
- 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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| 12. |
- 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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| 13. |
- 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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| 14. |
- Lutman, A. A., et al.
(författare)
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Polarization control in an X-ray free-electron laser
- 2016
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Ingår i: Nature Photonics. - : Springer Science and Business Media LLC. - 1749-4885 .- 1749-4893. ; 10:7, s. 468-472
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Tidskriftsartikel (refereegranskat)abstract
- X-ray free-electron lasers are unique sources of high-brightness coherent radiation. However, existing devices supply only linearly polarized light, precluding studies of chiral dynamics. A device called the Delta undulator has been installed at the Linac Coherent Light Source (LCLS) to provide tunable polarization. With a reverse tapered planar undulator line to pre-microbunch the beam and the novel technique of beam diverting, hundreds of microjoules of circularly polarized X-ray pulses are produced at 500-1,200 eV. These X-ray pulses are tens of femtoseconds long, have a degree of circular polarization of 0.98(+0.02)(-0.04) at 707 eV and may be scanned in energy. We also present a new two-colour X-ray pump-X-ray probe operating mode for the LCLS. Energy differences of Delta E/E = 2.4% are supported, and the second pulse can be adjusted to any elliptical polarization. In this mode, the pointing, timing, intensity and wavelength of the two pulses can be modified.
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| 15. |
- Rohringer, N., et al.
(författare)
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Stimulated X-Ray Raman Scattering with Free-Electron Laser Sources
- 2016
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Ingår i: X-Ray Lasers 2014. - Cham : Springer. - 0930-8989. - 9783319195216 - 9783319195209 ; , s. 201-207
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Bokkapitel (refereegranskat)abstract
- Stimulated electronic x-ray Raman scattering is the building block for several proposed x-ray pump probe techniques, that would allow the study of electron dynamics at unprecedented timescales.We present high spectral resolution data on stimulated electronic x-ray Raman scattering in a gas sample of neon using a self-amplified spontaneous emission x-ray free-electron laser. Despite the limited spectral coherence and broad bandwidth of these sources, high-resolution spectra can be obtained by statistical methods, opening the path to coherent stimulated x-ray Raman spectroscopy. An extension of these ideas to molecules and the results of a recent experiment in CO are discussed.
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| 16. |
- Varvarezos, Lazaros, et al.
(författare)
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Near-threshold two-photon double ionization of Kr in the vacuum ultraviolet
- 2021
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Ingår i: Physical Review A. - 2469-9926. ; 103:2
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Tidskriftsartikel (refereegranskat)abstract
- We report angle-resolved measurements on photoelectrons emitted upon near-threshold two-photon double ionization (TPDI) of Kr irradiated by free-electron laser (FEL) pulses. These photoelectron angular distributions (PADs) are compared with the results of semirelativistic R-matrix calculations. As reported by Augustin et al. [Phys. Rev. A 98, 033408 (2018)10.1103/PhysRevA.98.033408], it is found that the presence of autoionizing resonances within the bandwidth of the exciting FEL pulse strongly influences the PADs. In contrast to measurements on lower-Z targets such as Ne and Ar, the larger spin-orbit interaction, inherent in 4p-subshell hole states of Kr, permits us to resolve and study PADs associated with some of the fine-structure components of the Kr+ and Kr2+ ions.
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