| 1. |
- Squibb, Richard J., et al.
(författare)
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Acetylacetone photodynamics at a seeded free-electron laser
- 2018
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 9
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Tidskriftsartikel (refereegranskat)abstract
- Thefirst steps in photochemical processes, such as photosynthesis or animal vision, involvechanges in electronic and geometric structure on extremely short time scales. Time-resolvedphotoelectron spectroscopy is a natural way to measure such changes, but has been hinderedhitherto by limitations of available pulsed light sources in the vacuum-ultraviolet and soft X-ray spectral region, which have insufficient resolution in time and energy simultaneously. Theunique combination of intensity, energy resolution, and femtosecond pulse duration of theFERMI-seeded free-electron laser can now provide exceptionally detailed information onphotoexcitation–deexcitation and fragmentation in pump-probe experiments on the 50-femtosecond time scale. For the prototypical system acetylacetone we report here electronspectra measured as a function of time delay with enough spectral and time resolution tofollow several photoexcited species through well-characterized individual steps, interpretedusing state-of-the-art static and dynamics calculations. These results open the way forinvestigations of photochemical processes in unprecedented detail.
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| 2. |
- Asmussen, J. D., et al.
(författare)
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Time-Resolved Ultrafast Interatomic Coulombic Decay in Superexcited Sodium-Doped Helium Nanodroplets
- 2022
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Ingår i: Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185. ; 13:20, s. 4470-4478
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Tidskriftsartikel (refereegranskat)abstract
- The autoionization dynamics of super excited superfluid He nanodropletsdoped with Na atoms is studied by extreme-ultraviolet (XUV) time-resolved electronspectroscopy. Following excitation into the higher-lying droplet absorption band, the dropletrelaxes into the lowest metastable atomic 1s2s1,3Sstates from which interatomic Coulombicdecay (ICD) takes place either between two excited He atoms or between an excited He atomand a Na atom attached to the droplet surface. Four main ICD channels are identified, andtheir decay times are determined by varying the delay between the XUV pulse and a UV pulsethat ionizes the initial excited state and thereby quenches ICD. The decay times for thedifferent channels all fall in the range of similar to 1 ps, indicating that the ICD dynamics are mainlydetermined by the droplet environment. A periodic modulation of the transient ICD signals istentatively attributed to the oscillation of the bubble forming around the localized Heexcitation
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| 3. |
- Ceolin, Denis, et al.
(författare)
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Site-selective resonant Auger spectroscopy of iso-dichloroethylene at the carbon K-edge
- 2012
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Ingår i: Journal of Electron Spectroscopy and Related Phenomena. - : Elsevier BV. - 0368-2048 .- 1873-2526. ; 185:8-9, s. 252-258
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Tidskriftsartikel (refereegranskat)abstract
- This study focuses on the two C1s-to-LUMO (lowest unoccupied molecular orbital) excitations of the iso-dichloroethylene (H2C=CCl2) and the subsequent Auger decay. We investigate the effect of the two different carbon core excitations on the population of the cation produced after electronic relaxation. The resonant Auger spectra are interpreted by comparison to the valence shells photoionization spectrum and with the help of theoretical calculations. Several consequences of the core-hole localization on the electronic decay are observed. In particular, the resonant excitation of the C1s(CH2) to the LUMO leads to a large intensity increase in the region of the first satellite state, whereas no dramatic changes are observed for the C1s(CCl2) excitation.
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| 4. |
- Iwayama, H., et al.
(författare)
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A local chemical environment effect in site-specific Auger spectra of ethyl trifluoroacetate
- 2013
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 138:2, s. 024306-
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Tidskriftsartikel (refereegranskat)abstract
- We have investigated a local chemical environment effect on Auger spectra of ethyl trifluoroacetate (C4H5F3O2), using multi-electron coincidence spectroscopy and high-resolution electron spectroscopy. Site-specific KVV Auger spectra for each carbon atom, and for the fluorine and oxygen atoms are presented. The extent of hole localization in the final dicationic states was investigated with the help of theoretical calculations based on a two-hole population analysis. The Auger spectra have been simulated using a statistical approach. It is found that all Auger decays populate mainly localized dicationic states, with the two holes located either on the same fluorine atom or on adjacent fluorine atoms. While the decay of the F 1s hole populates exclusively the former states, the latter class of states is also populated by the decay of the C and O 1s holes.
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| 5. |
- Marchenko, T., et al.
(författare)
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Potential Energy Surface Reconstruction and Lifetime Determination of Molecular Double-Core-Hole States in the Hard X-Ray Regime
- 2017
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Ingår i: Physical Review Letters. - : AMER PHYSICAL SOC. - 0031-9007 .- 1079-7114. ; 119:13
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Tidskriftsartikel (refereegranskat)abstract
- A combination of resonant inelastic x-ray scattering and resonant Auger spectroscopy provides complementary information on the dynamic response of resonantly excited molecules. This is exemplified for CH3I, for which we reconstruct the potential energy surface of the dissociative I 3d(-2) double-core-hole state and determine its lifetime. The proposed method holds a strong potential for monitoring the hard x-ray induced electron and nuclear dynamic response of core-excited molecules containing heavy elements, where ab initio calculations of potential energy surfaces and lifetimes remain challenging.
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| 6. |
- Travnikova, O., et al.
(författare)
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Subfemtosecond Control of Molecular Fragmentation by Hard X-Ray Photons
- 2017
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Ingår i: Physical Review Letters. - : AMER PHYSICAL SOC. - 0031-9007 .- 1079-7114. ; 118:21
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Tidskriftsartikel (refereegranskat)abstract
- Tuning hard x-ray excitation energy along Cl 1s -> sigma* resonance in gaseous HCl allows manipulating molecular fragmentation in the course of the induced multistep ultrafast dissociation. The observations are supported by theoretical modeling, which shows a strong interplay between the topology of the potential energy curves, involved in the Auger cascades, and the so-called core-hole clock, which determines the time spent by the system in the very first step. The asymmetric profile of the fragmentation ratios reflects different dynamics of nuclear wave packets dependent on the photon energy.
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