| 1. |
- De Angelis, D., et al.
(författare)
-
A sub-100 nm thickness flat jet for extreme ultraviolet to soft X-ray absorption spectroscopy
- 2024
-
Ingår i: Journal of Synchrotron Radiation. - : International Union of Crystallography (IUCr). - 0909-0495 .- 1600-5775. ; 31:3 Pt, s. 605-612
-
Tidskriftsartikel (refereegranskat)abstract
- Experimental characterization of the structural, electronic and dynamic properties of dilute systems in aqueous solvents, such as nanoparticles, molecules and proteins, are nowadays an open challenge. X-ray absorption spectroscopy (XAS) is probably one of the most established approaches to this aim as it is element-specific. However, typical dilute systems of interest are often composed of light elements that require extreme-ultraviolet to soft X-ray photons. In this spectral regime, water and other solvents are rather opaque, thus demanding radical reduction of the solvent volume and removal of the liquid to minimize background absorption. Here, we present an experimental endstation designed to operate a liquid flat jet of sub-micrometre thickness in a vacuum environment compatible with extreme ultraviolet/soft XAS measurements in transmission geometry. The apparatus developed can be easily connected to synchrotron and free-electron-laser user-facility beamlines dedicated to XAS experiments. The conditions for stable generation and control of the liquid flat jet are analyzed and discussed. Preliminary soft XAS measurements on some test solutions are shown.
|
|
| 2. |
- Finetti, P., et al.
(författare)
-
Pulse duration of seeded free electron lasers
- 2017
-
Ingår i: Physical Review X. - 2160-3308. ; 7:2
-
Tidskriftsartikel (refereegranskat)abstract
- The pulse duration, and, more generally, the temporal intensity profile of free-electron laser (FEL) pulses, is of utmost importance for exploring the new perspectives offered by FELs; it is a nontrivial experimental parameter that needs to be characterized. We measured the pulse shape of an extreme ultraviolet externally seeded FEL operating in high-gain harmonic generation mode. Two different methods based on the cross-correlation of the FEL pulses with an external optical laser were used. The two methods, one capable of single-shot performance, may both be implemented as online diagnostics in FEL facilities. The measurements were carried out at the seeded FEL facility FERMI. The FEL temporal pulse characteristics were measured and studied in a range of FEL wavelengths and machine settings, and they were compared to the predictions of a theoretical model. The measurements allowed a direct observation of the pulse lengthening and splitting at saturation, in agreement with the proposed theory.
|
|
| 3. |
- Maznev, A. A., et al.
(författare)
-
Generation and detection of 50 GHz surface acoustic waves by extreme ultraviolet pulses
- 2021
-
Ingår i: Applied Physics Letters. - : AIP Publishing. - 0003-6951 .- 1077-3118. ; 119:4
-
Tidskriftsartikel (refereegranskat)abstract
- We use femtosecond extreme ultraviolet pulses derived from a free electron laser to excite and probe surface acoustic waves (SAWs) on the (001) surface of single crystal SrTiO3. SAWs are generated by a pair of 39.9 nm pulses crossed at the sample with the crossing angle defining the SAW wavelength at 84 nm. Detection of SAWs is performed via diffraction of a time-delayed 13.3 nm probe pulse by SAW-induced surface ripples. Despite the low reflectivity of the sample in the extreme ultraviolet range, the reflection mode detection is found to be efficient because of an increase in the diffraction efficiency for shorter wavelengths. We describe a methodology for extracting the SAW attenuation in the presence of a thermal grating, which is based on measuring the decay of oscillations at twice the SAW frequency. The proposed approach can be used to study ultrahigh frequency SAWs in a broad range of materials and will bridge the wave vector gap in surface phonon spectroscopy between Brillouin scattering and He atom scattering.
|
|
| 4. |
- von Korff Schmising, C., et al.
(författare)
-
Imaging Non-Local Magnetization Dynamics
- 2016
-
Ingår i: Synchrotron Radiation News. - : Informa UK Limited. - 0894-0886 .- 1931-7344. ; 29:3, s. 26-31
-
Tidskriftsartikel (refereegranskat)abstract
- Many fundamental processes in magnetism take place on a nanometer length and sub-picosecond time scale. An important example of such phenomena in magnetism is ultrafast, spin-polarized transport of laser-excited hot electrons, which is now being recognized as playing a crucial role for novel spintronic devices and for optically induced magnetic switching. Recent experimental examples include the demonstration of all-optical helicity dependent control of spin-polarized currents at interfaces [1], the design of novel and efficient terahertz emitters [2], and nanoscale spin reversal in chemically heterogeneous GdFeCo driven by non-local transfer of angular momentum [3]. In particular, for advanced information technologies with bit densities already exceeding 1 terabit per square inch with bit cell dimensions of (15 × 38 nm2) [4], it is of fundamental importance to understand and eventually control the mechanisms responsible for optically induced spin dynamics on the nanoscale.
|
|
| 5. |
- 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.
|
|
| 6. |
- LaRue, Jerry, et al.
(författare)
-
Symmetry-resolved CO desorption and oxidation dynamics on O/Ru(0001) probed at the C K-edge by ultrafast x-ray spectroscopy
- 2022
-
Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 157:16
-
Tidskriftsartikel (refereegranskat)abstract
- We report on carbon monoxide desorption and oxidation induced by 400 nm femtosecond laser excitation on the O/Ru(0001) surface probed by time-resolved x-ray absorption spectroscopy (TR-XAS) at the carbon K-edge. The experiments were performed under constant background pressures of CO (6 × 10−8 Torr) and O2 (3 × 10−8 Torr). Under these conditions, we detect two transient CO species with narrow 2π* peaks, suggesting little 2π* interaction with the surface. Based on polarization measurements, we find that these two species have opposing orientations: (1) CO favoring a more perpendicular orientation and (2) CO favoring a more parallel orientation with respect to the surface. We also directly detect gas-phase CO2 using a mass spectrometer and observe weak signatures of bent adsorbed CO2 at slightly higher x-ray energies than the 2π* region. These results are compared to previously reported TR-XAS results at the O K-edge, where the CO background pressure was three times lower (2 × 10−8 Torr) while maintaining the same O2 pressure. At the lower CO pressure, in the CO 2π* region, we observed adsorbed CO and a distribution of OC–O bond lengths close to the CO oxidation transition state, with little indication of gas-like CO. The shift toward “gas-like” CO species may be explained by the higher CO exposure, which blocks O adsorption, decreasing O coverage and increasing CO coverage. These effects decrease the CO desorption barrier through dipole–dipole interaction while simultaneously increasing the CO oxidation barrier.
|
|
| 7. |
- Pedersoli, E., et al.
(författare)
-
Mesoscale morphology of airborne core-shell nanoparticle clusters : x-ray laser coherent diffraction imaging
- 2013
-
Ingår i: Journal of Physics B. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 46:16 SI, s. 164033-
-
Tidskriftsartikel (refereegranskat)abstract
- Unraveling the complex morphology of functional materials like core-shell nanoparticles and its evolution in different environments is still a challenge. Only recently has the single-particle coherent diffraction imaging (CDI), enabled by the ultrabright femtosecond free-electron laser pulses, provided breakthroughs in understanding mesoscopic morphology of nanoparticulate matter. Here, we report the first CDI results for Co@SiO2 core-shell nanoparticles randomly clustered in large airborne aggregates, obtained using the x-ray free-electron laser at the Linac Coherent Light Source. Our experimental results compare favourably with simulated diffraction patterns for clustered Co@SiO2 nanoparticles with similar to 10 nm core diameter and similar to 30 nm shell outer diameter, which confirms the ability to resolve the mesoscale morphology of complex metastable structures. The findings in this first morphological study of core-shell nanomaterials are a solid base for future time-resolved studies of dynamic phenomena in complex nanoparticulate matter using x-ray lasers.
|
|
| 8. |
- Sala, Simone, et al.
(författare)
-
Pulse-to-pulse wavefront sensing at free-electron lasers using ptychography
- 2020
-
Ingår i: Journal of applied crystallography. - : INT UNION CRYSTALLOGRAPHY. - 0021-8898 .- 1600-5767. ; 53, s. 949-956
-
Tidskriftsartikel (refereegranskat)abstract
- The pressing need for knowledge of the detailed wavefront properties of ultra-bright and ultra-short pulses produced by free-electron lasers has spurred the development of several complementary characterization approaches. Here a method based on ptychography is presented that can retrieve high-resolution complex-valued wavefunctions of individual pulses without strong constraints on the illumination or sample object used. The technique is demonstrated within experimental conditions suited for diffraction experiments and exploiting Kirkpatrick-Baez focusing optics. This lensless technique, applicable to many other short-pulse instruments, can achieve diffraction-limited resolution.
|
|
| 9. |
- Schmising, C. von Korff, et al.
(författare)
-
Imaging Ultrafast Demagnetization Dynamics after a Spatially Localized Optical Excitation
- 2014
-
Ingår i: Physical Review Letters. - 1079-7114. ; 111:21
-
Tidskriftsartikel (refereegranskat)abstract
- Ultrashort, coherent x-ray pulses of a free-electron laser are used to holographically image the magnetization dynamics within a magnetic domain pattern after creation of a localized excitation via an optical standing wave. We observe a spatially confined reduction of the magnetization within a couple of hundred femtoseconds followed by its slower recovery. Additionally, the experimental results show evidence of a spatial evolution of magnetization, which we attribute to ultrafast transport of nonequilibrium spin-polarized electrons for early times and to a fluence-dependent remagnetization rate for later times.
|
|
| 10. |
- Schreck, Simon, et al.
(författare)
-
Atom-Specific Probing of Electron Dynamics in an Atomic Adsorbate by Time-Resolved X-Ray Spectroscopy
- 2022
-
Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 129:27
-
Tidskriftsartikel (refereegranskat)abstract
- The electronic excitation occurring on adsorbates at ultrafast timescales from optical lasers that initiate surface chemical reactions is still an open question. Here, we report the ultrafast temporal evolution of x-ray absorption spectroscopy (XAS) and x-ray emission spectroscopy (XES) of a simple well-known adsorbate prototype system, namely carbon (C) atoms adsorbed on a nickel [Ni(100)] surface, following intense laser optical pumping at 400 nm. We observe ultrafast (∼100 fs) changes in both XAS and XES showing clear signatures of the formation of a hot electron-hole pair distribution on the adsorbate. This is followed by slower changes on a few picoseconds timescale, shown to be consistent with thermalization of the complete C/Ni system. Density functional theory spectrum simulations support this interpretation.
|
|
