| 1. |
- Cryan, J P, et al.
(författare)
-
Molecular frame Auger electron energy spectrum from N2
- 2012
-
Ingår i: Journal of Physics B. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 45:5, s. 055601-
-
Tidskriftsartikel (refereegranskat)abstract
- Here we present the first angle-resolved, non-resonant (normal) Auger spectra for impulsively aligned nitrogen molecules. We have measured the angular pattern of Auger electron emission following K -shell photoionization by 1.1 keV photons from the Linac Coherent Light Source (LCLS). Using strong-field-induced molecular alignment to make molecular frame measurements is equally effective for both repulsive and quasi-bound final states. The capability to resolve Auger emission angular distributions in the molecular frame of reference provides a new tool for spectral assignments in congested Auger electron spectra that takes advantage of the symmetries of the final diction states. Based on our experimental results and theoretical predictions, we propose the assignment of the spectral features in the Auger electron spectrum.
|
|
| 2. |
- Mazza, T., et al.
(författare)
-
Mapping Resonance Structures in Transient Core-Ionized Atoms
- 2020
-
Ingår i: Physical Review X. - 2160-3308. ; 10:4
-
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.
|
|
| 3. |
- Sanchez-Gonzalez, A., et al.
(författare)
-
Accurate prediction of X-ray pulse properties from a free-electron laser using machine learning
- 2017
-
Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 8
-
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.
|
|
| 4. |
- Berrah, N., et al.
(författare)
-
Femtosecond-resolved observation of the fragmentation of buckminsterfullerene following X-ray multiphoton ionization
- 2019
-
Ingår i: Nature Physics. - : Springer Science and Business Media LLC. - 1745-2473 .- 1745-2481. ; 15, s. 1279-1283
-
Tidskriftsartikel (refereegranskat)abstract
- X-ray free-electron lasers have, over the past decade, opened up the possibility of understanding the ultrafast response of matter to intense X-ray pulses. In earlier research on atoms and small molecules, new aspects of this response were uncovered, such as rapid sequences of inner-shell photoionization and Auger ionization. Here, we studied a larger molecule, buckminsterfullerene (C60), exposed to 640eV X-rays, and examined the role of chemical effects, such as chemical bonds and charge transfer, on the fragmentation following multiple ionization of the molecule. To provide time resolution, we performed femtosecond-resolved X-ray pump/X-ray probe measurements, which were accompanied by advanced simulations. The simulations and experiment reveal that despite substantial ionization induced by the ultrashort (20fs) X-ray pump pulse, the fragmentation of C60 is considerably delayed. This work uncovers the persistence of the molecular structure of C60, which hinders fragmentation over a timescale of hundreds of femtoseconds. Furthermore, we demonstrate that a substantial fraction of the ejected fragments are neutral carbon atoms. These findings provide insights into X-ray free-electron laser-induced radiation damage in large molecules, including biomolecules.
|
|
| 5. |
- Bilodeau, R. C., et al.
(författare)
-
High-charge-state formation following inner-shell photodetachment from S-
- 2005
-
Ingår i: Physical Review A. - 1050-2947. ; 72, s. 050701-
-
Tidskriftsartikel (refereegranskat)abstract
- The formation of S+, S2+, S3+, and S4+ is observed following inner-shell photodetachment of S–. The photodetachment spectra for all possible ionic products are obtained over a large region of photon energies covering both the 2p and 2s thresholds (S5+, is energetically allowed at the higher photon energies, but not observed), and are placed on an absolute scale. The 2s threshold energy is measured to be 224.6(5) eV, allowing the determination of the neutral atomic S 2s–13s23p5 inner-shell excited state energy for the first time. The S– 2s–13s23p6 2S1/2 state is observed as a Feshbach resonance 2.3(5) eV below the 2s threshold in the S+, S2+, and S3+ product channels.
|
|
| 6. |
- Cryan, James P., et al.
(författare)
-
Auger Electron Angular Distribution of Double Core-Hole States in the Molecular Reference Frame
- 2010
-
Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 105:8, s. 083004-
-
Tidskriftsartikel (refereegranskat)abstract
- The Linac Coherent Light Source free electron laser is a source of high brightness x rays, 2×1011 photons in a ∼5 fs pulse, that can be focused to produce double core vacancies through rapid sequential ionization. This enables double core vacancy Auger electron spectroscopy, an entirely new way to study femtosecond chemical dynamics with Auger electrons that probe the local valence structure of molecules near a specific atomic core. Using 1.1 keV photons for sequential x-ray ionization of impulsively aligned molecular nitrogen, we observed a rich single-site double core vacancy Auger electron spectrum near 413 eV, in good agreement with ab initio calculations, and we measured the corresponding Auger electron angle dependence in the molecular frame.
|
|
| 7. |
- Frasinski, L. J., et al.
(författare)
-
Dynamics of Hollow Atom Formation in Intense X-Ray Pulses Probed by Partial Covariance Mapping
- 2013
-
Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 111:7, s. 073002-
-
Tidskriftsartikel (refereegranskat)abstract
- When exposed to ultraintense x-radiation sources such as free electron lasers (FELs) the innermost electronic shell can efficiently be emptied, creating a transient hollow atom or molecule. Understanding the femtosecond dynamics of such systems is fundamental to achieving atomic resolution in flash diffraction imaging of noncrystallized complex biological samples. We demonstrate the capacity of a correlation method called partial covariance mapping'' to probe the electron dynamics of neon atoms exposed to intense 8 fs pulses of 1062 eV photons. A complete picture of ionization processes competing in hollow atom formation and decay is visualized with unprecedented ease and the map reveals hitherto unobserved nonlinear sequences of photoionization and Auger events. The technique is particularly well suited to the high counting rate inherent in FEL experiments.
|
|
| 8. |
- Glownia, James M., et al.
(författare)
-
Time-resolved pump-probe experiments at the LCLS
- 2010
-
Ingår i: Optics Express. - 1094-4087. ; 18:17, s. 17620-17630
-
Tidskriftsartikel (refereegranskat)abstract
- The first time-resolved x-ray/optical pump-probe experiments at the SLAC Linac Coherent Light Source (LCLS) used a combination of feedback methods and post-analysis binning techniques to synchronize an ultrafast optical laser to the linac-based x-ray laser. Transient molecular nitrogen alignment revival features were resolved in time-dependent x-ray-induced fragmentation spectra. These alignment features were used to find the temporal overlap of the pump and probe pulses. The strong-field dissociation of x-ray generated quasi-bound molecular dications was used to establish the residual timing jitter. This analysis shows that the relative arrival time of the Ti:Sapphire laser and the x-ray pulses had a distribution with a standard deviation of approximately 120 fs. The largest contribution to the jitter noise spectrum was the locking of the laser oscillator to the reference RF of the accelerator, which suggests that simple technical improvements could reduce the jitter to better than 50 fs.
|
|
| 9. |
|
|
| 10. |
- McFarland, B. K., et al.
(författare)
-
Ultrafast X-ray Auger probing of photoexcited molecular dynamics
- 2014
-
Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 5, s. 4235-
-
Tidskriftsartikel (refereegranskat)abstract
- Molecules can efficiently and selectively convert light energy into other degrees of freedom. Disentangling the underlying ultrafast motion of electrons and nuclei of the photoexcited molecule presents a challenge to current spectroscopic approaches. Here we explore the photoexcited dynamics of molecules by an interaction with an ultrafast X-ray pulse creating a highly localized core hole that decays via Auger emission. We discover that the Auger spectrum as a function of photoexcitation-X-ray-probe delay contains valuable information about the nuclear and electronic degrees of freedom from an element-specific point of view. For the nucleobase thymine, the oxygen Auger spectrum shifts towards high kinetic energies, resulting from a particular C-O bond stretch in the pi pi* photoexcited state. A subsequent shift of the Auger spectrum towards lower kinetic energies displays the electronic relaxation of the initial photoexcited state within 200 fs. Ab-initio simulations reinforce our interpretation and indicate an electronic decay to the n pi* state.
|
|
| 11. |
- Mucke, Melanie, et al.
(författare)
-
Covariance mapping of two-photon double core hole states in C2H2 and C2H6 produced by an x-ray free electron laser
- 2015
-
Ingår i: New Journal of Physics. - : IOP Publishing. - 1367-2630. ; 17
-
Tidskriftsartikel (refereegranskat)abstract
- Few-photon ionization and relaxation processes in acetylene (C2H2) and ethane (C2H6) were investigated at the linac coherent light source x-ray free electron laser (FEL) at SLAC, Stanford using a highly efficient multi-particle correlation spectroscopy technique based on a magnetic bottle. The analysis method of covariance mapping has been applied and enhanced, allowing us to identify electron pairs associated with double core hole (DCH) production and competing multiple ionization processes including Auger decay sequences. The experimental technique and the analysis procedure are discussed in the light of earlier investigations of DCH studies carried out at the same FEL and at third generation synchrotron radiation sources. In particular, we demonstrate the capability of the covariance mapping technique to disentangle the formation of molecular DCH states which is barely feasible with conventional electron spectroscopy methods.
|
|
| 12. |
- Saleacuten, P., et al.
(författare)
-
X-ray FEL-induced Double Core-Hole Formation in Polyatomic Molecules
- 2012
-
Ingår i: Journal of Physics, Conference Series. - : IOP Publishing. - 1742-6588 .- 1742-6596. ; 388:2, s. 022083-
-
Tidskriftsartikel (refereegranskat)abstract
- We use extremely intense, ultrashort soft X-Ray pulses generated by the LCLS X-Ray Free Electron Laser to investigate the production of molecular double core-hole states by sequential two-photon X-Ray absorption. The effect of critical LCLS parameters such as the number of photons per pulse, the pulse duration, and the focal spot size on the photoelectron and Auger spectra is modeled in detail and the results of these simulations are used as an aid in the interpretation of the experimental spectra obtained. The emphasis is on double core-hole formation in small polyatomic molecules such as CO2.
|
|
| 13. |
- Sanchez-Gonzalez, A., et al.
(författare)
-
Auger electron and photoabsorption spectra of glycine in the vicinity of the oxygen K-edge measured with an X-FEL
- 2015
-
Ingår i: Journal of Physics B-Atomic Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 48:23
-
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.
|
|
| 14. |
- Takanashi, T, et al.
(författare)
-
Time-Resolved Measurement of Interatomic Coulombic Decay Induced by Two-Photon Double Excitation of Ne2
- 2017
-
Ingår i: Physical Review Letters. - 0031-9007. ; 118:3
-
Tidskriftsartikel (refereegranskat)abstract
- The hitherto unexplored two-photon doubly excited states [Ne∗(2p-13s)]2 were experimentally identified using the seeded, fully coherent, intense extreme ultraviolet free-electron laser FERMI. These states undergo ultrafast interatomic Coulombic decay (ICD), which predominantly produces singly ionized dimers. In order to obtain the rate of ICD, the resulting yield of Ne2+ ions was recorded as a function of delay between the extreme ultraviolet pump and UV probe laser pulses. The extracted lifetimes of the long-lived doubly excited states, 390(-130/+450) fs, and of the short-lived ones, less than 150 fs, are in good agreement with ab initio quantum mechanical calculations.
|
|
| 15. |
- Thomas, H., et al.
(författare)
-
Explosions of Xenon Clusters in Ultraintense Femtosecond X-Ray Pulses from the LCLS Free Electron Laser
- 2012
-
Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 108:13
-
Tidskriftsartikel (refereegranskat)abstract
- Explosions of large Xe clusters (< N > similar to 11 000) irradiated by femtosecond pulses of 850 eV x-ray photons focused to an intensity of up to 1017 W/cm(2) from the Linac Coherent Light Source were investigated experimentally. Measurements of ion charge-state distributions and energy spectra exhibit strong evidence for the formation of a Xe nanoplasma in the intense x-ray pulse. This x-ray produced Xe nanoplasma is accompanied by a three-body recombination and hydrodynamic expansion. These experimental results appear to be consistent with a model in which a spherically exploding nanoplasma is formed inside the Xe cluster and where the plasma temperature is determined by photoionization heating.
|
|
| 16. |
|
|
| 17. |
- Zhaunerchyk, Vitali, et al.
(författare)
-
Disentangling formation of multiple-core holes in aminophenol molecules exposed to bright X-FEL radiation
- 2015
-
Ingår i: Journal of Physics B. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 48:24
-
Tidskriftsartikel (refereegranskat)abstract
- Competing multi-photon ionization processes, some leading to the formation of double core hole states, have been examined in 4-aminophenol. The experiments used the linac coherent light source (LCLS) x-ray free electron laser, in combination with a time-of-flight magnetic bottle electron spectrometer and the correlation analysis method of covariance mapping. The results imply that 4-aminophenol molecules exposed to the focused x-ray pulses of the LCLS sequentially absorb more than two x-ray photons, resulting in the formation of multiple core holes as well as in the sequential removal of photoelectrons and Auger electrons (so-called PAPA sequences).
|
|
| 18. |
- Zhaunerchyk, Vitali, et al.
(författare)
-
Using covariance mapping to investigate the dynamics of multi-photon ionization processes of Ne atoms exposed to X-FEL pulses
- 2013
-
Ingår i: Journal of Physics B. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 46:16, s. 164034-
-
Tidskriftsartikel (refereegranskat)abstract
- We report on a detailed investigation into the electron emission processes of Ne atoms exposed to intense femtosecond x-ray pulses, provided by the Linac Coherent Light Source Free Electron Laser (FEL) at Stanford. The covariance mapping technique is applied to analyse the data, and the capability of this approach to disentangle both linear and nonlinear correlation features which may be hidden on coincidence maps of the same data set is demonstrated. Different correction techniques which enable improvements on the quality of the spectral features extracted from the covariance maps are explored. Finally, a method for deriving characteristics of the x-ray FEL pulses based on covariance mapping in combination with model simulations is presented.
|
|
| 19. |
- Barillot, T., et al.
(författare)
-
Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule
- 2021
-
Ingår i: Physical Review X. - : American Physical Society. - 2160-3308. ; 11:3
-
Tidskriftsartikel (refereegranskat)abstract
- The possibility of suddenly ionized molecules undergoing extremely fast electron hole (or hole) dynamics prior to significant structural change was first recognized more than 20 years ago and termed charge migration. The accurate probing of ultrafast electron hole dynamics requires measurements that have both sufficient temporal resolution and can detect the localization of a specific hole within the molecule. We report an investigation of the dynamics of inner valence hole states in isopropanol where we use an x-ray pump-x-ray probe experiment, with site and state-specific probing of a transient hole state localized near the oxygen atom in the molecule, together with an ab initio theoretical treatment. We record the signature of transient hole dynamics and make the first tentative observation of dynamics driven by frustrated Auger-Meitner transitions. We verify that the effective hole lifetime is consistent with our theoretical prediction. This state-specific measurement paves the way to widespread application for observations of transient hole dynamics localized in space and time in molecules and thus to charge transfer phenomena that are fundamental in chemical and material physics.
|
|
| 20. |
- Berrah, Nora, et al.
(författare)
-
Double-core-hole spectroscopy for chemical analysis with an intense X-ray femtosecond laser
- 2011
-
Ingår i: Proceedings of the National Academy of Sciences of the United States of America. - : Proceedings of the National Academy of Sciences. - 0027-8424 .- 1091-6490. ; 108:41, s. 16912-16915
-
Tidskriftsartikel (refereegranskat)abstract
- Theory predicts that double-core-hole (DCH) spectroscopy can provide a new powerful means of differentiating between similar chemical systems with a sensitivity not hitherto possible. Although DCH ionization on a single site in molecules was recently measured with double-and single-photon absorption, double-core holes with single vacancies on two different sites, allowing unambiguous chemical analysis, have remained elusive. Here we report that direct observation of double-core holes with single vacancies on two different sites produced via sequential two-photon absorption, using short, intense X-ray pulses from the Linac Coherent Light Source free-electron laser and compare it with theoretical modeling. The observation of DCH states, which exhibit a unique signature, and agreement with theory proves the feasibility of the method. Our findings exploit the ultrashort pulse duration of the free-electron laser to eject two core electrons on a time scale comparable to that of Auger decay and demonstrate possible future X-ray control of physical inner-shell processes.
|
|
| 21. |
- Bolognesi, P., et al.
(författare)
-
A study of the dynamical energy flow in uracil
- 2015
-
Ingår i: Journal of Physics, Conference Series. - : IOP Publishing. - 1742-6588 .- 1742-6596. ; 635
-
Tidskriftsartikel (refereegranskat)abstract
- The time resolved photoionization of C 1s in uracil following excitation of the neutral molecule by 260 nm pulses has been studied at LCLS.
|
|
| 22. |
- Fang, L., et al.
(författare)
-
Multiple Ionization and Double Core-hole Production in Molecules using the LCLS X-ray FEL
- 2012
-
Ingår i: Journal of Physics, Conference Series. - : IOP Publishing. - 1742-6588 .- 1742-6596. ; 388:3, s. 032028-
-
Tidskriftsartikel (refereegranskat)abstract
- We used the world's first hard x-ray FEL to investigate the response of molecular systems to the ultra-intense, femtosecond x-ray radiation. We report sequential multiphoton ionization, frustrated absorption and double core hole production mechanisms.
|
|
| 23. |
- Farrell, J. P., et al.
(författare)
-
Ultrafast X-ray probe of nucleobase photoprotection
- 2012
-
Ingår i: Quantum Electronics and Laser Science Conference. - 9781467318396 ; , s. 6327153-
-
Konferensbidrag (refereegranskat)abstract
- We will present first results of a UV-pump X-ray-probe study of the photoprotection mechanism of thymine. The experiment used element specific Auger spectroscopy and was carried out at the LCLS.
|
|
| 24. |
- Iablonskyi, D., et al.
(författare)
-
Interatomic Coulombic Decay Processes after Multiple Valence Excitations in Ne Clusters
- 2015
-
Ingår i: Journal of Physics: Conference Series. - : IOP Publishing. - 1742-6596 .- 1742-6588. ; 635, s. 112067-112067
-
Konferensbidrag (refereegranskat)abstract
- We present a comprehensive analysis of autoionization processes in Ne clusters (similar to 5000 atoms) after multiple valence excitations by free electron laser radiation. The evolution from 2-body interatomic Coulombic decay (ICD) to 3-body ICD is demonstrated when changing from surface to bulk Frenkel exciton excitation. Super Coster-Kronig type 2-body ICD is observed at Wannier exciton which quenches the main ICD channel.
|
|
| 25. |
- Iablonskyi, D., et al.
(författare)
-
Slow Interatomic Coulombic Decay of Multiply Excited Neon Clusters
- 2016
-
Ingår i: Physical Review Letters. - 0031-9007. ; 117:27
-
Tidskriftsartikel (refereegranskat)abstract
- Ne clusters (∼5000 atoms) were resonantly excited (2p→3s) by intense free electron laser (FEL) radiation at FERMI. Such multiply excited clusters can decay nonradiatively via energy exchange between at least two neighboring excited atoms. Benefiting from the precise tunability and narrow bandwidth of seeded FEL radiation, specific sites of the Ne clusters were probed. We found that the relaxation of cluster surface atoms proceeds via a sequence of interatomic or intermolecular Coulombic decay (ICD) processes while ICD of bulk atoms is additionally affected by the surrounding excited medium via inelastic electron scattering. For both cases, cluster excitations relax to atomic states prior to ICD, showing that this kind of ICD is rather slow (picosecond range). Controlling the average number of excitations per cluster via the FEL intensity allows a coarse tuning of the ICD rate.
|
|
| 26. |
- Ilchen, M., et al.
(författare)
-
X-ray spectroscopy on ultrafast-decaying core-excited atomic ions
- 2020
-
Ingår i: Charge-exchange. - : IOP Publishing. - 1742-6588. ; 1412
-
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.
|
|
| 27. |
- Larsson, Mats, et al.
(författare)
-
Double core-hole formation in small molecules at the LCLS free electron laser
- 2013
-
Ingår i: Journal of Physics B. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 46:16, s. 164030-
-
Tidskriftsartikel (refereegranskat)abstract
- We have investigated nonlinear processes in small molecules by x-ray photoelectron spectroscopy using the Linac Coherent Light Source free electron laser, and by simulations. The main focus of the experiments was the formation of the two-site double core-hole (tsDCH) states in the molecules CO2, N2O and N-2. These experiments are described in detail and the results are compared with simulations of the photoelectron spectra. The double core-hole states, and in particular the tsDCH states, have been predicted to be highly sensitive to the chemical environment. The theory behind this chemical sensitivity is validated by the experiments. Furthermore, our simulations of the relative integrated intensities of the peaks associated with the nonlinear processes show that this type of simulation, in combination with experimental data, provides a useful tool for estimating the duration of ultra-short x-ray pulses.
|
|
| 28. |
- McFarland, B. K., et al.
(författare)
-
Probing nucleobase photoprotection with soft x-rays
- 2013
-
Ingår i: XVIIITH INTERNATIONAL CONFERENCE ON ULTRAFAST PHENOMENA. - : EDP Sciences. - 9782759809561 ; , s. 07004-
-
Konferensbidrag (refereegranskat)abstract
- Nucleobases absorb strongly in the ultraviolet region, leading to molecular excitation into reactive states. The molecules avoid the photoreactions by funnelling the electronic energy into less reactive states on an ultrafast timescale via non-Born-Oppenheimer dynamics. Current theory on the nucleobase thymine discusses two conflicting pathways for the photoprotective dynamics. We present our first results of our free electron laser based UV-pump soft x-ray-probe study of the photoprotection mechanism of thymine. We use the high spatial sensitivity of the Auger electrons emitted after the soft x-ray pulse induced core ionization. Our transient spetra show two timescales on the order of 200 fs and 5 ps, in agreement with previous (all UV) ultrafast experiments. The timescales appear at different Auger kinetic energies which will help us to decipher the molecular dynamics.
|
|
| 29. |
- Murphy, B. F., et al.
(författare)
-
Femtosecond X-ray-induced explosion of C-60 at extreme intensity
- 2014
-
Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 5
-
Tidskriftsartikel (refereegranskat)abstract
- Understanding molecular femtosecond dynamics under intense X-ray exposure is critical to progress in biomolecular imaging and matter under extreme conditions. Imaging viruses and proteins at an atomic spatial scale and on the time scale of atomic motion requires rigorous, quantitative understanding of dynamical effects of intense X-ray exposure. Here we present an experimental and theoretical study of C-60 molecules interacting with intense X-ray pulses from a free-electron laser, revealing the influence of processes not previously reported. Our work illustrates the successful use of classical mechanics to describe all moving particles in C-60, an approach that scales well to larger systems, for example, biomolecules. Comparisons of the model with experimental data on C-60 ion fragmentation show excellent agreement under a variety of laser conditions. The results indicate that this modelling is applicable for X-ray interactions with any extended system, even at higher X-ray dose rates expected with future light sources.
|
|
| 30. |
- Sahlén, Martin, et al.
(författare)
-
Experimental Verification of the Chemical Sensitivity of Two-Site Double Core-Hole States Formed by an X-Ray Free-Electron Laser
- 2012
-
Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 108:15, s. 153003-
-
Tidskriftsartikel (refereegranskat)abstract
- We have performed x-ray two-photon photoelectron spectroscopy using the Linac Coherent Light Source x-ray free-electron laser in order to study double core-hole (DCH) states of CO2, N2O, and N-2. The experiment verifies the theory behind the chemical sensitivity of two-site DCH states by comparing a set of small molecules with respect to the energy shift of the two-site DCH state and by extracting the relevant parameters from this shift.
|
|
| 31. |
- Ueda, Kiyoshi, et al.
(författare)
-
Roadmap on photonic, electronic and atomic collision physics : I. Light-matter interaction
- 2019
-
Ingår i: Journal of Physics B. - : IOP PUBLISHING LTD. - 0953-4075 .- 1361-6455. ; 52:17
-
Tidskriftsartikel (refereegranskat)abstract
- We publish three Roadmaps on photonic, electronic and atomic collision physics in order to celebrate the 60th anniversary of the ICPEAC conference. In Roadmap I, we focus on the light-matter interaction. In this area, studies of ultrafast electronic and molecular dynamics have been rapidly growing, with the advent of new light sources such as attosecond lasers and x-ray free electron lasers. In parallel, experiments with established synchrotron radiation sources and femtosecond lasers using cutting-edge detection schemes are revealing new scientific insights that have never been exploited. Relevant theories are also being rapidly developed. Target samples for photon-impact experiments are expanding from atoms and small molecules to complex systems such as biomolecules, fullerene, clusters and solids. This Roadmap aims to look back along the road, explaining the development of these fields, and look forward, collecting contributions from twenty leading groups from the field.
|
|
| 32. |
- Wehlitz, R, et al.
(författare)
-
Photon energy dependence of ionization-excitation in helium at medium energies
- 1997
-
Ingår i: Journal of Physics B: Atomic, Molecular and Optical Physics. - 0953-4075. ; 30:2, s. L51-L58
-
Tidskriftsartikel (refereegranskat)abstract
- We have measured the photoionization-excitation-to-photoionization ratio for He(+)nl (n = 2-6) at several photon energies from 90 to 900 eV. By extrapolating these values we could determine the asymptotic high-energy ratios for He(+)nl (n = 2-5) which agree with theoretical predictions. We show that the satellite-to-main-line ratios are consistent with experimental double-to-single photoionization ratios and agree well with recent measurements.
|
|
| 33. |
- Wolf, T. J. A., et al.
(författare)
-
Probing molecular photoinduced dynamics by ultrafast soft x-rays
- 2017
-
Ingår i: 2017 Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC). 25-29 June 2017, Munich, Germany. - : IEEE. - 9781509067367 - 9781509067374
-
Konferensbidrag (refereegranskat)abstract
- Summary form only given. Molecules selectively transform light energy from the sun into other forms of energy like heat, electricity, or chemical energy with high quantum efficiency. The energy conversion process is the result of a correlated motion of electrons and nuclei after photoexcitation, often under breakdown of the Born-Oppenheimer approximation. The element and site selectivity of x-rays allows observing molecular processes from a different point of view compared to ultrafast optical probes [1,2]. I will concentrate on time resolved x-ray absorption spectroscopy. The method provides high selectivity on the transient electronic structure of a molecule. Recently, we establishes this method in the soft x-ray domain for probing ππ* to nπ* transitions, a general and important process for molecular energy conversion. Fig. 1 shows a sketch of thymine, used in the experiment, with one of the oxygen 1s core orbitals and the π,n and π* valence orbitals. While valence orbitals are generally delocalized over the whole molecular body, the lone pair n orbital is essentially an oxygen 2p orbital. An x-ray induced transition from the oxygen 1s to the n orbital will result in a strong absorption maximum in the pre-edge region. We use this feature to probe the molecular dynamics after photoexcitation.
|
|
| 34. |
- Wolf, T.J.A., et al.
(författare)
-
Probing ultrafast ππ*/nπ* internal conversion in organic chromophores via K-edge resonant absorption
- 2017
-
Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 8:1
-
Tidskriftsartikel (refereegranskat)abstract
- Many photoinduced processes including photosynthesis and human vision happen in organic molecules and involve coupled femtosecond dynamics of nuclei and electrons. Organic molecules with heteroatoms often possess an important excited-state relaxation channel from an optically allowed ππ* to a dark nπ* state. The ππ*/nπ* internal conversion is difficult to investigate, as most spectroscopic methods are not exclusively sensitive to changes in the excited-state electronic structure. Here, we report achieving the required sensitivity by exploiting the element and site specificity of near-edge soft X-ray absorption spectroscopy. As a hole forms in the n orbital during ππ*/nπ* internal conversion, the absorption spectrum at the heteroatom K-edge exhibits an additional resonance. We demonstrate the concept using the nucleobase thymine at the oxygen K-edge, and unambiguously show that ππ*/nπ* internal conversion takes place within (60 ± 30) fs. High-level-coupled cluster calculations confirm the method’s impressive electronic structure sensitivity for excited-state investigations.
|
|
| 35. |
- Wolf, T.J.A., et al.
(författare)
-
Transient Resonant Auger-Meitner Spectra of Photoexcited Thymine
- 2021
-
Ingår i: Faraday discussions. - : Royal Society of Chemistry (RSC). - 1364-5498 .- 1359-6640. ; 228, s. 555-70
-
Tidskriftsartikel (refereegranskat)abstract
- We present the first investigation of excited state dynamics by resonant Auger-Meitner spectroscopy (also known as resonant Auger spectroscopy) using the nucleobase thymine as an example. Thymine is photoexcited in the UV and probed with X-ray photon energies at and below the oxygen K-edge. After initial photoexcitation to a ππ* excited state, thymine is known to undergo internal conversion to an nπ* excited state with a strong resonance at the oxygen K-edge, red-shifted from the groundstate π* resonances of thymine (see our previous study Wolf et al.,Nat. Commun., 2017,8, 29). We resolve and compare the Auger-Meitner electron spectra associated both with the excited state and ground state resonances, and distinguish participato rand spectator decay contributions. Furthermore, we observe simultaneously with the decay of the nπ* state signatures the appearance of additional resonant Auger-Meitner contributions at photon energies between the nπ* state and the ground state resonances. We assign these contributions to population transfer from the nπ* state to a ππ* triplet state via intersystem crossing on the picosecond timescale based on simulations of the X-ray absorption spectra in the vibrationally hot triplet state. Moreover, we identify signatures from the initially excited ππ* singlet state which we have not observed in our previous study.
|
|
