| 1. |
- Gisselbrecht, Mathieu, et al.
(författare)
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Size dependent fragmentation of argon clusters in the soft x-ray ionization regime.
- 2008
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 128:4
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Tidskriftsartikel (refereegranskat)abstract
- Photofragmentation of argon clusters of average size ranging from 10 up to 1000 atoms is studied using soft x-ray radiation below the 2p threshold and multicoincidence mass spectroscopy technique. For small clusters (N=10), ionization induces fast fragmentation with neutral emission imparting a large amount of energy. While the primary dissociation takes place on a picosecond time scale, the fragments undergo slow degradation in the spectrometer on a microsecond time scale. For larger clusters (N>/=100) we believe that we observe the fragmentation pattern of multiply charged species on a time-scale which lasts a few hundred nanoseconds. The reason for these slower processes is the large number of neutral atoms which act as an efficient cooling bath where the excess energy ("heat") dissipates among all degrees of freedom. Further degradation of the photoionic cluster in spectrometer then takes place on the microsecond time scale, similar to small clusters.
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| 2. |
- Arnold, Cord L., et al.
(författare)
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A high-repetition rate attosecond pulse source for coincidence spectroscopy
- 2021
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Ingår i: 2021 Conference on Lasers and Electro-Optics Europe and European Quantum Electronics Conference, CLEO/Europe-EQEC 2021. - 9781665418768
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Konferensbidrag (refereegranskat)abstract
- The power of attosecond pump-probe spectroscopy combined with advanced detection schemes, such as photoelectron/ion coincidence spectrometers and time-resolved photoelectron emission microscopy (PEEM), can be unleashed by properly accounting for the repetition rate of the source. In this work, we present a high-repetition rate (200 kHz) attosecond pulse source that opens up for exploring phenomena, previously inaccessible to the community using attosecond interferometric and spectroscopy pump-probe techniques [1].
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| 3. |
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| 4. |
- Barillot, T., et al.
(författare)
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Angular asymmetry and attosecond time delay from the giant plasmon resonance in C60 photoionization
- 2015
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Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 91
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Tidskriftsartikel (refereegranskat)abstract
- This combined experimental and theoretical study demonstrates that the surface plasmon resonance in C 60 alters the valence photoemission quantum phase, resulting in strong effects in the photoelectron angular distribution and emission time delay. Electron momentum imaging spectroscopy is used to measure the photoelectron angular distribution asymmetry parameter that agrees well with our calculations from the time-dependent local density approximation (TDLDA). Significant structure in the valence photoemission time delay is simultaneously calculated by TDLDA over the plasmon active energies. Results reveal a unified spatial and temporal asymmetry pattern driven by the plasmon resonance and offer a sensitive probe of electron correlation. A semiclassical approach facilitates further insights into this link that can be generalized and applied to other molecular systems and nanometer-sized metallic materials exhibiting plasmon resonances.
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| 5. |
- Barillot, T., et al.
(författare)
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Attosecond time delays in C-60 valence photoemissions at the giant plasmon
- 2015
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Ingår i: Journal of Physics: Conference Series. - : IOP Publishing. - 1742-6596 .- 1742-6588. ; 635, s. 112074-112074
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Konferensbidrag (refereegranskat)abstract
- We perform time-dependent local density functional calculations of the time delay in C-60 HOMO and HOMO-1 photoionization at giant plasmon energies. A semiclassical model is used to develop further insights.
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| 6. |
- Busto, David, et al.
(författare)
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Fano's Propensity Rule in Angle-Resolved Attosecond Pump-Probe Photoionization
- 2019
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Ingår i: Physical Review Letters. - : AMER PHYSICAL SOC. - 0031-9007 .- 1079-7114. ; 123:13
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Tidskriftsartikel (refereegranskat)abstract
- In a seminal article, Fano predicts that absorption of light occurs preferably with increase of angular momentum. We generalize Fano's propensity rule to laser-assisted photoionization, consisting of absorption of an extreme-ultraviolet photon followed by absorption or emission of an infrared photon. The predicted asymmetry between absorption and emission leads to incomplete quantum interference in attosecond photoelectron interferometry. It explains both the angular dependence of the photoionization time delays and the delay dependence of the photoelectron angular distributions. Our theory is verified by experimental results in Ar in the 20-40 eV range.
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| 7. |
- Busto, David, et al.
(författare)
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Probing electronic decoherence with high-resolution attosecond photoelectron interferometry
- 2022
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Ingår i: European Physical Journal D. - : Springer Science and Business Media LLC. - 1434-6060 .- 1434-6079. ; 76:7
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Tidskriftsartikel (refereegranskat)abstract
- Abstract: Quantum coherence plays a fundamental role in the study and control of ultrafast dynamics in matter. In the case of photoionization, entanglement of the photoelectron with the ion is a well-known source of decoherence when only one of the particles is measured. Here, we investigate decoherence due to entanglement of the radial and angular degrees of freedom of the photoelectron. We study two-photon ionization via the 2s2p autoionizing state in He using high spectral resolution photoelectron interferometry. Combining experiment and theory, we show that the strong dipole coupling of the 2s2p and 2p2 states results in the entanglement of the angular and radial degrees of freedom. This translates, in angle-integrated measurements, into a dynamic loss of coherence during autoionization. Graphic Abstract: [Figure not available: see fulltext.]. © 2022, The Author(s).
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| 8. |
- Carlström, Stefanos, et al.
(författare)
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Quantum coherence in photo-ionisation with tailored XUV pulses
- 2018
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Ingår i: Journal of Physics B: Atomic, Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 51:1
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Tidskriftsartikel (refereegranskat)abstract
- Ionisation with ultrashort pulses in the extreme ultraviolet (XUV) regime can be used to prepare an ion in a superposition of spin-orbit substates. In this work, we study the coherence properties of such a superposition, created by ionising xenon atoms using two phase-locked XUV pulses at different frequencies. In general, if the duration of the driving pulse exceeds the quantum beat period, dephasing will occur. If however, the frequency difference of the two pulses matches the spin-orbit splitting, the coherence can be efficiently increased and dephasing does not occur.
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| 9. |
- Cheng, Yu Chen, et al.
(författare)
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Controlling photoionization using attosecond time-slit interferences
- 2020
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Ingår i: Proceedings of the National Academy of Sciences of the United States of America. - : Proceedings of the National Academy of Sciences. - 0027-8424. ; 117:20, s. 10727-10732
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Tidskriftsartikel (refereegranskat)abstract
- When small quantum systems, atoms or molecules, absorb a high-energy photon, electrons are emitted with a well-defined energy and a highly symmetric angular distribution, ruled by energy quantization and parity conservation. These rules are based on approximations and symmetries which may break down when atoms are exposed to ultrashort and intense optical pulses. This raises the question of their universality for the simplest case of the photoelectric effect. Here we investigate photoionization of helium by a sequence of attosecond pulses in the presence of a weak infrared laser field. We continuously control the energy of the photoelectrons and introduce an asymmetry in their emission direction, at variance with the idealized rules mentioned above. This control, made possible by the extreme temporal confinement of the light-matter interaction, opens a road in attosecond science, namely, the manipulation of ultrafast processes with a tailored sequence of attosecond pulses.
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| 10. |
- Cheng, Yu Chen, et al.
(författare)
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Imaging multiphoton ionization dynamics of CH3I at a high repetition rate XUV free-electron laser
- 2021
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Ingår i: Journal of Physics B-Atomic Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 54:1
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Tidskriftsartikel (refereegranskat)abstract
- XUV multiphoton ionization of molecules is commonly used in free-electron laser experiments to study charge transfer dynamics. However, molecular dissociation and electron dynamics, such as multiple photon absorption, Auger decay, and charge transfer, often happen on competing time scales, and the contributions of individual processes can be difficult to unravel. We experimentally investigate the Coulomb explosion dynamics of methyl iodide upon core-hole ionization of the shallow inner-shell of iodine (4d) and classically simulate the fragmentation by phenomenologically introducing ionization dynamics and charge transfer. Under our experimental conditions with medium fluence and relatively long XUV pulses (similar to 75 fs), we find that fast Auger decay prior to charge transfer significantly contributes to the charging mechanism, leading to a yield enhancement of higher carbon charge states upon molecular dissociation. Furthermore, we argue for the existence of another charging mechanism for the weak fragmentation channels leading to triply charged carbon atoms. This study shows that classical simulations can be a useful tool to guide the quantum mechanical description of the femtosecond dynamics upon multiphoton absorption in molecular systems.
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| 11. |
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| 12. |
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| 13. |
- Dahlström, J. Marcus, 1982-, et al.
(författare)
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Theory of attosecond delays in laser-assisted photoionization
- 2013
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Ingår i: Chemical Physics. - : Elsevier BV. - 0301-0104 .- 1873-4421. ; 414, s. 53-64
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Tidskriftsartikel (refereegranskat)abstract
- We study the temporal aspects of laser-assisted extreme ultraviolet (XUV) photoionization using attosecond pulses of harmonic radiation. The aim of this paper is to establish the general form of the phase of the relevant transition amplitudes and to make the connection with the time-delays that have been recently measured in experiments. We find that the overall phase contains two distinct types of contributions: one is expressed in terms of the phase-shifts of the photoelectron continuum wavefunction while the other is linked to continuum–continuum transitions induced by the infrared (IR) laser probe. Our formalism applies to both kinds of measurements reported so far, namely the ones using attosecond pulse trains of XUV harmonics and the others based on the use of isolated attosecond pulses (streaking). The connection between the phases and the time-delays is established with the help of finite difference approximations to the energy derivatives of the phases. The observed time-delay is a sum of two components: a one-photon Wigner-like delay and an universal delay that originates from the probing process itself.
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| 14. |
- Dahlström, Marcus, et al.
(författare)
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Atomic and macroscopic measurements of attosecond pulse trains
- 2009
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Ingår i: Physical Review A (Atomic, Molecular and Optical Physics). - 1050-2947. ; 80:3
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Tidskriftsartikel (refereegranskat)abstract
- We characterize attosecond pulses in a train using both the well established "reconstruction of attosecond beating by interference of two-photon transitions" (RABITT) technique and the recently demonstrated in situ method, which is based on a weak perturbation of the harmonic generation process by the second harmonic of the laser field. The latter technique determines the characteristics of the single atom emission, while RABITT allows one to measure attosecond pulses "on target." By comparing the results of the two methods, the influence of propagation and filtering on the attosecond pulses can be extracted.
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| 15. |
- Erny, Christian, et al.
(författare)
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Metrology of high-order harmonics for free-electron laser seeding
- 2011
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Ingår i: New Journal of Physics. - : IOP Publishing. - 1367-2630. ; 13
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Tidskriftsartikel (refereegranskat)abstract
- We examine the characteristics of high-order harmonics generated with 800 nm, 25 mJ, 160 fs laser pulses in an Ar gas cell with the objective of seeding a free electron laser. We measure the energy per pulse and per harmonic, the energy jitter, the divergence and the position stability of the harmonic beam. We perform ab initio numerical simulations based on integration of the time-dependent Schrodinger equation and of the wave equation within the slowly varying envelope approximation. The results reproduce the experimental measurements to better than a factor of two. The interaction of a frequency comb of harmonic fields with an electron bunch in an undulator is examined with a simple model consisting of calculating the energy modulation owing to the seed-electron interaction. The model indicates that the undulator acts as a spectral filter selecting a given harmonic.
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| 16. |
- Feifel, Raimund, et al.
(författare)
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From localised to delocalised electronic states in free Ar, Kr and Xe clusters
- 2004
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Ingår i: European Physical Journal D. Atomic, Molecular, Optical and Plasma Physics. - : Springer Science and Business Media LLC. - 1434-6060 .- 1434-6079. ; 30:3, s. 343-351
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Tidskriftsartikel (refereegranskat)abstract
- We present new results for the inner valence levels of clusters of the three inert gases Ar, Kr and Xe based on photoelectron spectroscopy studies. The inner valence levels are compared to the localised core levels and to the delocalised outer valence levels. This comparison shows a gradual change from a relatively localised behaviour for Ar inner valence 3s, over the intermediate case of Kr inner valence 4s, to a more delocalised behaviour for Xe inner valence 5s. This change correlates well with the ratio between the orbital sizes and the interatomic distances. The Kr4s intermediate case is found to exhibit characteristics of both localised and delocalised behaviour.
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| 17. |
- Ganguly, Smita, et al.
(författare)
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Coincidence study of core-ionized adamantane: Site-sensitivity within a carbon cage?
- 2022
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Ingår i: Physical chemistry chemical physics : PCCP. - 1463-9084. ; 24:47, s. 28994-29003
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Tidskriftsartikel (refereegranskat)abstract
- We investigate the fragmentation dynamics of adamantane dications produced after core-ionization at the carbon edge followed by Auger decay. The combination of high-resolution electron spectroscopy, energy-resolved electron-ion multi-coincidence spectroscopy and different theoretical models allows us to give a complete characterization of the processes involved after ionization. We show that energy- and site-sensitivity is observed even for a highly-symmetric molecule that lacks any unique atomic site.
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| 18. |
- Ganguly, Smita, et al.
(författare)
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Resonant Inner-Shell Photofragmentation of Adamantane (C10H16)
- 2023
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Ingår i: Molecules. - 1420-3049. ; 28:14
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Tidskriftsartikel (refereegranskat)abstract
- Adamantane, the smallest diamondoid molecule with a symmetrical cage, contains two distinct carbon sites, CH and CH2. The ionization/excitation of the molecule leads to the cage opening and strong structural reorganization. While theoretical predictions suggest that the carbon site CH primarily causes the cage opening, the role of the other CH2 site remains unclear. In this study, we used advanced experimental Auger electron-ion coincidence techniques and theoretical calculations to investigate the fragmentation dynamics of adamantane after resonant inner-shell photoexcitation. Our results demonstrate that some fragmentation channels exhibit site-sensitivity of the initial core-hole location, indicating that different carbon site excitations could lead to unique cage opening mechanisms.
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| 19. |
- Ganguly, Smita, et al.
(författare)
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The origin of enhanced O2+ production from photoionized CO2 clusters
- 2022
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Ingår i: Communications Chemistry. - 2399-3669.
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Tidskriftsartikel (refereegranskat)abstract
- CO2-rich planetary atmospheres are continuously exposed to ionising radiation driving major photochemical processes. In the Martian atmosphere, CO2 clusters are predicted to exist at high altitudes motivating a deeper understanding of their photochemistry. In this joint experimental-theoretical study, we investigate the photoreactions of CO2 clusters (≤2 nm) induced by soft X-ray ionisation. We observe dramatically enhanced production of O2- from photoionized CO2 clusters compared to the case of the isolated molecule and identify two relevant reactions. Using quantum chemistry calculations and multi-coincidence mass spectrometry, we pinpoint the origin of this enhancement: A size-dependent structural transition of the clusters from a covalently bonded arrangement to a weakly bonded polyhedral geometry that activates an exothermic reaction producing O+2. Our results unambiguously demonstrate that the photochemistry of small clusters/particles will likely have a strong influence on the ion balance in atmospheres.
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| 20. |
- Gisselbrecht, Mathieu, et al.
(författare)
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Charge migration and decay of doubly charged ammonia clusters
- 2012
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Ingår i: Journal of Physics, Conference Series. - : IOP Publishing. - 1742-6588 .- 1742-6596. ; 388:2, s. 022112-
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Tidskriftsartikel (refereegranskat)abstract
- The photo-fragmentation of ammonia molecular clusters ionized with soft x-rays is studied for photon energies near the N-1s threshold. The fragmentation is studied with a 3D momentum mass spectrometer to access the energy and angular correlations between fragments. By choosing the cluster sizes below or above the critical size of stable dication, we investigate the coulomb explosion dynamics and the interplay between charge delocalization and mobility of molecules in the clusters.
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| 21. |
- Gisselbrecht, Mathieu, et al.
(författare)
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Exploring single-photon ionization on the attosecond time scale
- 2012
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Ingår i: XXVII International Conference on Photonic, Electronic and Atomic Collisions (Icpeac 2011), Pts 1-15. - : IOP Publishing. - 1742-6588 .- 1742-6596. ; 388, s. 032025-032025
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Konferensbidrag (refereegranskat)abstract
- One of the fundamental processes in nature is the photoelectric effect in which an electron is ripped away from its atom via the interaction with a photon. This process was long believed to be instantaneous but with the development of attosecond pulses (1 as 10(-18) s) we can finally get an insight into its dynamic. Here we measure a delay in ionization time between two differently bound electrons. The outgoing electrons are created via ionization with a train of attosecond pulses and we probe their relative delay with a synchronized infrared laser. We demonstrate how this probe field influences the measured delays and show that this contribution can be estimated with a universal formula, which allows us to extract field free atomic data..
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| 22. |
- Gisselbrecht, Mathieu, et al.
(författare)
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Photon energy dependence of fragmentation of small argon clusters
- 2005
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 123:19
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Tidskriftsartikel (refereegranskat)abstract
- Photofragmentation of small argon clusters with size below ten atoms is reported. In this size range significant modifications from the electronic properties and geometry take place. When tuning the photon energy through the argon 2p edge, the fragmentation pattern is changed. Specifically, cation dimer production is enhanced at the 2p(3/2)-> 4s resonance, while above the 2p edge almost complete atomization is observed. In both cases, the widths of the peaks in the mass spectra indicate that a large amount of kinetic energy is imparted to the fragment due to the formation of multiply charged clusters. A model based on "Coulomb explosion"-charge separation, simply resulting in a complete atomization of the cluster with no dependence on the photon energy-is insufficient to explain the observed photofragmentation of small clusters.
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| 23. |
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| 24. |
- Guenot, Diego, et al.
(författare)
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Measurements of relative photoemission time delays in noble gas atoms
- 2014
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Ingår i: Journal of Physics B. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 47:24, s. 245602-
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Tidskriftsartikel (refereegranskat)abstract
- We determine relative photoemission time delays between valence electrons in different noble gas atoms (Ar, Ne and He) in an energy range between 31 and 37 eV. The atoms are ionized by an attosecond pulse train synchronized with an infrared laser field and the delays are measured using an interferometric technique. We compare our results with calculations using the random phase approximation with exchange and multi-configurational Hartree-Fock. We also investigate the influence of the different ionization angular channels.
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| 25. |
- Guenot, Diego, et al.
(författare)
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Photoemission time delay measurements and calculations close to the 3s ionization cross section minimum in ar
- 2012
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Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 85:5, s. 053424-
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Tidskriftsartikel (refereegranskat)abstract
- We present experimental measurements and theoretical calculations of photoionization time delays from the 3s and 3p shells in Ar in the photon energy range of 32-42 eV. The experimental measurements are performed by interferometry using attosecond pulse trains and the infrared laser used for their generation. The theoretical approach includes intershell correlation effects between the 3s and 3p shells within the framework of the random-phase approximation with exchange. The connection between single-photon ionization and the two-color two-photon ionization process used in the measurement is established using the recently developed asymptotic approximation for the complex transition amplitudes of laser-assisted photoionization. We compare and discuss the theoretical and experimental results, especially in the region where strong intershell correlations in the 3s -> kp channel lead to an induced Cooper minimum in the 3s ionization cross section.
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