| 1. |
- Berrah, N., et al.
(författare)
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Femtosecond-resolved observation of the fragmentation of buckminsterfullerene following X-ray multiphoton ionization
- 2019
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Ingår i: Nature Physics. - : Springer Science and Business Media LLC. - 1745-2473 .- 1745-2481. ; 15, s. 1279-1283
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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.
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| 2. |
- Bilodeau, R. C., et al.
(författare)
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High-charge-state formation following inner-shell photodetachment from S-
- 2005
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Ingår i: Physical Review A. - 1050-2947. ; 72, s. 050701-
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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.
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| 3. |
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| 4. |
- Fang, L., et al.
(författare)
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Multiple Ionization and Double Core-hole Production in Molecules using the LCLS X-ray FEL
- 2012
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Ingår i: Journal of Physics, Conference Series. - : IOP Publishing. - 1742-6588 .- 1742-6596. ; 388:3, s. 032028-
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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.
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| 5. |
- Frasinski, L. J., et al.
(författare)
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Dynamics of Hollow Atom Formation in Intense X-Ray Pulses Probed by Partial Covariance Mapping
- 2013
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Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 111:7, s. 073002-
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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.
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| 6. |
- Kosugi, S., et al.
(författare)
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Conjugate photoelectron recapture peaks in the high resolution Auger electron spectra following near-threshold Ar 2p photoionization
- 2020
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Ingår i: Journal of Physics B. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 53:12
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Tidskriftsartikel (refereegranskat)abstract
- We have observed formation of Rydberg series superimposed on the Ar (L3M2,3M2,3) Auger electron spectral profile with photoexcitation just above the 2p(3/2)(-1) photoionization threshold. This is due to the recapture of photoelectrons induced by post-collision interaction between the Auger electron and photoelectron: Ar+ 2p(3/2)(-1) + e(-) -> Ar+ 3p(-2)ml + e(-). The intensity distribution of the angular momentum state resolved Rydberg peaks revealed prominent conjugate peaks due to angular momentum exchange between photoelectrons and Auger electrons in the process. In addition, we measured the 2p(3/2)(-1)nl -> 3p(-2)ml + e(-) resonant Auger spectra with high resolution below the 2p(3/2)(-1) threshold. Our results showed that conjugate shake-up/down 2p(3/2)(-1)nd -> 3p(-2)mp + e(-) processes are stronger than the direct 2p(3/2)(-1)nd -> 3p(-2)ms, (m-1)d + e(-) processes in the spectator Auger processes, implying a strong angular momentum exchange effect between photoelectron and Auger electron.
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| 7. |
- Kosugi, S., et al.
(författare)
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Strong configuration interaction in the 3p photoelectron spectrum of Kr
- 2020
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Ingår i: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - 2469-9926 .- 2469-9934. ; 101:4
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Tidskriftsartikel (refereegranskat)abstract
- We measured the Kr photoelectron spectrum in the region close to the 3p ionization threshold. Our high-resolution measurements allowed a clear observation of spectral structures due to electron correlation effects. Analysis based on relativistic multiconfiguration calculations could explain these observed peaks as due to strong configuration interactions between the 3p(-1) state and 3d(-2) nl states. Calculated and experimental data for peak assignments and intensity distributions are in good agreement. In addition, we measured the anisotropy parameter beta, which also agreed well with theory. These findings provide a detailed view of strong configuration interactions between the 3(-1) and 3d(-2)nl inner-shell hole states.
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| 8. |
- Kukk, E., et al.
(författare)
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Formative period in the x-ray-induced photodissociation of organic molecules
- 2021
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Ingår i: Physical Review Research. - 2643-1564. ; 3:1
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Tidskriftsartikel (refereegranskat)abstract
- Absorption of x-ray photons by atomic inner shells of light-element organics and biomolecules often leads to formation of dicationic electronic states and to molecular fragmentation. We investigated the x-ray-induced dissociation landscape of a representative medium-sized organic molecule, thiophene, by femtosecond x-ray pulses from the Super Photon Ring-8 GeV (SPring-8) Angstrom Compact Free-Electron Laser (SACLA). Holes, created in the sulfur 2p orbital by photoemission, were filled by the Auger process that created dicationic molecular states within a broad range of internal energies—a starting point particular to x-ray-induced dynamics. The evolution of the ionized molecules was monitored by a pump-probe experiment using a near-infrared (800 nm) laser pulse. Ion-ion coincidence and ion momentum analysis reveals enhanced yields of ionic fragments from multibody breakup of the ring, attributed to additional ionization of the highly excited fraction of the dicationic parent molecular states. The transient nature of the enhancement and its decay with about a 160-fs time constant indicate formation of an open-ring parent geometry and the statistical survival time of the parent species before the dissociation events. By probing specific Auger final states of transient, highly excited nature by near-infrared light, we demonstrate how pump-probe signatures can be related to the key features in dynamics during the early period of the x-ray-induced damage of organic molecules and biomolecules.
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| 9. |
- Larsson, Mats, et al.
(författare)
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Double core-hole formation in small molecules at the LCLS free electron laser
- 2013
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Ingår i: Journal of Physics B. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 46:16, s. 164030-
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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.
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| 10. |
- Li, S., et al.
(författare)
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Manifestation of postcollision interaction in Krypton LMN Auger spectra following K-shell photoionization
- 2022
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Ingår i: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - : American Physical Society. - 2469-9926 .- 2469-9934. ; 106:2
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Tidskriftsartikel (refereegranskat)abstract
- We report on an experimental and theoretical study of postcollision interaction (PCI) effects on L-2 - M4,5N2,3 Auger electrons measured above the Kr K-edge in which L-2 vacancies are primarily generated by KL2 x-ray emission. Such cascade processes, in which a deep inner-shell vacancy decays first by x-ray emission followed by Auger electron emission, is a strong decay mode in heavy atoms. The L-2 - M4,5N2,3 Auger electron peak is observed to become increasingly asymmetric with a shifting peak maximum as the absorbed x-ray energy approaches the K-shell ionization threshold. This is attributed to PCI energy exchanges of the Auger electron with the 1s photoelectron. To model the PCI effects, we have applied a semiclassical approach modified to account for the combined lifetimes of the K and L-2 hole states. In addition, our analysis treats several closely spaced Auger transitions with final ionic states having different terms and angular momenta.
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