| 1. |
- Gahl, Cornelius, et al.
(författare)
-
A femtosecond X-ray/optical cross-correlator
- 2008
-
Ingår i: Nature Photonics. - : Springer Science and Business Media LLC. - 1749-4885 .- 1749-4893. ; 2:3, s. 165-169
-
Tidskriftsartikel (refereegranskat)abstract
- For a fundamental understanding of ultrafast dynamics in chemistry, biology and materials science it has been a long-standing dream to record a molecular movie in which both the atomic trajectories and the chemical states of every atom in matter are followed in real time(1). Free- electron lasers provide this perspective as they deliver brilliant femtosecond X-ray pulses spanning a wide photon energy range, which is necessary to gather element- specific and chemical- stateselective information with femtosecond time resolution. The key challenge lies in synchronizing the free- electron lasers with separate optical lasers. We exploit the peak brilliance of the free- electron laser in Hamburg(2,3) ( FLASH) and establish X- raypulseinduced transient changes of the optical reflectivity in GaAs as a powerful tool for X- ray/ optical cross- correlation. This constitutes a breakthrough in the path towards recording a molecular movie and - equally importantly - opens up the field of femtosecond X- ray- induced dynamics, only accessible with high- brilliance X- ray free- electron lasers.
|
|
| 2. |
- Thielemann-Kühn, Nele, et al.
(författare)
-
Optical control of 4f orbital state in rare-earth metals
- 2024
-
Ingår i: Science Advances. - : American Association for the Advancement of Science (AAAS). - 2375-2548. ; 10:16
-
Tidskriftsartikel (refereegranskat)abstract
- A change of orbital state alters the coupling between ions and their surroundings drastically. Orbital excitations are hence key to understand and control interaction of ions. Rare-earth elements with strong magneto-crystalline anisotropy (MCA) are important ingredients for magnetic devices. Thus, control of their localized 4f magnetic moments and anisotropy is one major challenge in ultrafast spin physics. With time-resolved x-ray absorption and resonant inelastic scattering experiments, we show for Tb metal that 4f-electronic excitations out of the ground-state multiplet occur after optical pumping. These excitations are driven by inelastic 5d-4f-electron scattering, altering the 4f-orbital state and consequently the MCA with important implications for magnetization dynamics in 4f-metals and more general for the excitation of localized electronic states in correlated materials.
|
|
| 3. |
- Beye, Martin, et al.
(författare)
-
Chemical Bond Activation Observed with an X-ray Laser
- 2016
-
Ingår i: Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185 .- 1948-7185. ; 7:18, s. 3647-3651
-
Tidskriftsartikel (refereegranskat)abstract
- The concept of bonding and antibonding orbitals is fundamental in chemistry. The population of those orbitals and the energetic difference between the two reflect the strength of the bonding interaction. Weakening the bond is expected to reduce this energetic splitting, but the transient character of bond-activation has so far prohibited direct experimental access. Here we apply time-resolved soft X-ray spectroscopy at a free electron laser to directly observe the decreased bonding antibonding splitting following bond-activation using an ultrashort optical laser pulse.
|
|
| 4. |
- Laksmono, Hartawan, et al.
(författare)
-
Anomalous Behavior of the Homogeneous Ice Nucleation Rate in No-Man's Land
- 2015
-
Ingår i: Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185 .- 1948-7185. ; 6:14, s. 2826-2832
-
Tidskriftsartikel (refereegranskat)abstract
- We present an analysis of ice nucleation kinetics from near-ambient pressure water as temperature decreases below the homogeneous limit T-H by cooling micrometer-sized droplets (microdroplets) evaporatively at 10(3)-10(4) K/s and probing the structure ultrafast using femtosecond pulses from the Linac Coherent Light Source (LCLS) free-electron X-ray laser. Below 232 K, we observed a slower nucleation rate increase with decreasing temperature than anticipated from previous measurements, which we suggest is due to the rapid decrease in water's diffusivity. This is consistent with earlier findings that microdroplets do not crystallize at <227 K, but vitrify at cooling rates of 10(6)-10(7) K/s. We also hypothesize that the slower increase in the nucleation rate is connected with the proposed fragile-to-strong transition anomaly in water.
|
|
| 5. |
- Lojewski, Tobias, et al.
(författare)
-
The interplay of local electron correlations and ultrafast spin dynamics in fcc Ni
- 2023
-
Ingår i: Materials Research Letters. - : Taylor & Francis. - 2166-3831. ; 11:8, s. 655-661
-
Tidskriftsartikel (refereegranskat)abstract
- The complex electronic structure of metallic ferromagnets is determined by a balance between exchange interaction, electron hopping leading to band formation, and local Coulomb repulsion. By combining high energy and temporal resolution in femtosecond time-resolved X-ray absorption spectroscopy with ab initio time-dependent density functional theory we analyze the electronic structure in fcc Ni on the time scale of these interactions in a pump-probe experiment. We distinguish transient broadening and energy shifts in the absorption spectra, which we demonstrate to be captured by electron repopulation respectively correlation-induced modifications of the electronic structure, requiring to take the local Coulomb interaction into account.
|
|
| 6. |
|
|
| 7. |
- Chergui, Majed, et al.
(författare)
-
Progress and prospects in nonlinear extreme-ultraviolet and X-ray optics and spectroscopy
- 2023
-
Ingår i: Nature reviews physics. - 2522-5820. ; :5, s. 578-596
-
Forskningsöversikt (refereegranskat)abstract
- Free-electron lasers and high-harmonic-generation table-top systems are new sources of extreme-ultraviolet to hard X-ray photons, providing ultrashort pulses that are intense, coherent and tunable. They are enabling a broad range of nonlinear optical and spectroscopic methods at short wavelengths, similar to those developed in the terahertz to ultraviolet regimes over the past 60 years. The extreme-ultraviolet to X-ray wavelengths access core transitions that can provide element and orbital selectivity, structural resolution down to the sub-nanometre scale and, for some methods, high momentum transfers across typical Brillouin zones; the possibilities for polarization control and sub-femtosecond time resolution are opening up new frontiers in research. In this Roadmap, we review the emergence of this field over the past 10 years or so, covering methods such as sum or difference frequency generation and second-harmonic generation, two-photon absorption, stimulated emission or Raman spectroscopy and transient grating spectroscopy. We then discuss the unique opportunities provided by these techniques for probing elementary dynamics in a wide variety of systems. X-ray free-electron lasers and high-harmonic-generation sources of extreme-ultraviolet (EUV) to hard X-ray photons deliver intense ultrashort pulses and enable the extension of nonlinear methods to much shorter wavelengths.EUV to X-ray wavelengths access core transitions that can provide element and orbital selectivity. These wavelengths also achieve sub-nanometre structural resolution and high momentum transfer, with femtosecond and attosecond time resolution.Nonlinear EUV/X-ray methods that have emerged include sum or difference frequency generation, parametric down-conversion, second-harmonic generation, two-photon absorption, stimulated emission or Raman spectroscopy and transient grating spectroscopy.Nonlinear EUV/X-ray science is developing hand-in-hand with instrumentation, to improve pulse features and enhance accessibility with the use of table-top systems or compact accelerators.These techniques offer unique opportunities for probing dynamical events in a wide variety of systems, including surface and interface processes, chirality, nanoscale transport and multidimensional core-level spectroscopy. New sources of extreme-ultraviolet to hard X-ray photons have enabled a wide range of short-wavelength nonlinear optical and spectroscopic methods over the past decade, and, for the future, offer unique opportunities to probe elementary dynamics in various systems.
|
|
| 8. |
- Diesen, Elias, et al.
(författare)
-
Ultrafast Adsorbate Excitation Probed with Subpicosecond-Resolution X-Ray Absorption Spectroscopy
- 2021
-
Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 127:1
-
Tidskriftsartikel (refereegranskat)abstract
- We use a pump-probe scheme to measure the time evolution of the C K-edge x-ray absorption spectrum from CO/Ru(0001) after excitation by an ultrashort high-intensity optical laser pulse. Because of the short duration of the x-ray probe pulse and precise control of the pulse delay, the excitation-induced dynamics during the first picosecond after the pump can be resolved with unprecedented time resolution. By comparing with density functional theory spectrum calculations, we find high excitation of the internal stretch and frustrated rotation modes occurring within 200 fs of laser excitation, as well as thermalization of the system in the picosecond regime. The ∼100 fs initial excitation of these CO vibrational modes is not readily rationalized by traditional theories of nonadiabatic coupling of adsorbates to metal surfaces, e.g., electronic frictions based on first order electron-phonon coupling or transient population of adsorbate resonances. We suggest that coupling of the adsorbate to nonthermalized electron-hole pairs is responsible for the ultrafast initial excitation of the modes.
|
|
| 9. |
- Eckert, Sebastian, et al.
(författare)
-
Ultrafast Independent N-H and N-C Bond Deformation Investigated with Resonant Inelastic X-Ray Scattering
- 2017
-
Ingår i: Angewandte Chemie International Edition. - : Wiley. - 1433-7851 .- 1521-3773. ; 56:22, s. 6088-6092
-
Tidskriftsartikel (refereegranskat)abstract
- The femtosecond excited-state dynamics following resonant photoexcitation enable the selective deformation of N-H and N-C chemical bonds in 2-thiopyridone in aqueous solution with optical or X-ray pulses. In combination with multiconfigurational quantum-chemical calculations, the orbital-specific electronic structure and its ultrafast dynamics accessed with resonant inelastic X-ray scattering at the N 1s level using synchrotron radiation and the soft X-ray free-electron laser LCLS provide direct evidence for this controlled photoinduced molecular deformation and its ultrashort time-scale.
|
|
| 10. |
- Engel, Robin Y., et al.
(författare)
-
Electron population dynamics in resonant non-linear x-ray absorption in nickel at a free-electron laser
- 2023
-
Ingår i: Structural Dynamics. - : American Institute of Physics (AIP). - 2329-7778. ; 10:5
-
Tidskriftsartikel (refereegranskat)abstract
- Free-electron lasers provide bright, ultrashort, and monochromatic x-ray pulses, enabling novel spectroscopic measurements not only with femtosecond temporal resolution: The high fluence of their x-ray pulses can also easily enter the regime of the non-linear x-ray-matter interaction. Entering this regime necessitates a rigorous analysis and reliable prediction of the relevant non-linear processes for future experiment designs. Here, we show non-linear changes in the L-3-edge absorption of metallic nickel thin films, measured with fluences up to 60 J/cm(2). We present a simple but predictive rate model that quantitatively describes spectral changes based on the evolution of electronic populations within the pulse duration. Despite its simplicity, the model reaches good agreement with experimental results over more than three orders of magnitude in fluence, while providing a straightforward understanding of the interplay of physical processes driving the non-linear changes. Our findings provide important insights for the design and evaluation of future high-fluence free-electron laser experiments and contribute to the understanding of non-linear electron dynamics in x-ray absorption processes in solids at the femtosecond timescale.
|
|
