| 1. |
- Luo, Sizuo, et al.
(författare)
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Ultra-stable and versatile high-energy resolution setup for attosecond photoelectron spectroscopy
- 2023
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Ingår i: Advances in Physics: X. - 2374-6149. ; 8:1
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Forskningsöversikt (refereegranskat)abstract
- Attosecond photoelectron spectroscopy has opened up for studying light–matter interaction on ultrafast time scales. It is often performed with interferometric experimental setups that require outstanding stability. We demonstrate and characterize in detail an actively stabilized, versatile, high spectral resolution attosecond beamline based on a Mach-Zehnder interferometer. The active stabilization keeps the interferometer ultra-stable for several hours with an RMS stability of 13 as and a total pump-probe delay scanning range of (Formula presented.) fs. A tunable femtosecond laser source to drive high-order harmonic generation allows for precisely addressing atomic and molecular resonances. Furthermore, the interferometer includes a spectral shaper in 4f-geometry in the probe arm as well as a tunable bandpass filter in the pump arm, which offer additional high flexibility in terms of tunability as well as narrowband or polychromatic probe pulses. We demonstrate the capabilities of the beamline via experiments using several variants of the RABBIT (reconstruction of attosecond beating by two photon transitions) technique. In this setup, the temporal-spectral resolution of photoelectron spectroscopy can reach a new level of accuracy and precision.
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| 2. |
- Young, Linda, et al.
(författare)
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Roadmap of ultrafast x-ray atomic and molecular physics
- 2018
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Ingår i: Journal of Physics B: Atomic, Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 51:3
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Forskningsöversikt (refereegranskat)abstract
- X-ray free-electron lasers (XFELs) and table-top sources of x-rays based upon high harmonic generation (HHG) have revolutionized the field of ultrafast x-ray atomic and molecular physics, largely due to an explosive growth in capabilities in the past decade. XFELs now provide unprecedented intensity (1020 W cm-2) of x-rays at wavelengths down to ∼1 Ångstrom, and HHG provides unprecedented time resolution (∼50 attoseconds) and a correspondingly large coherent bandwidth at longer wavelengths. For context, timescales can be referenced to the Bohr orbital period in hydrogen atom of 150 attoseconds and the hydrogen-molecule vibrational period of 8 femtoseconds; wavelength scales can be referenced to the chemically significant carbon K-edge at a photon energy of ∼280 eV (44 Ångstroms) and the bond length in methane of ∼1 Ångstrom. With these modern x-ray sources one now has the ability to focus on individual atoms, even when embedded in a complex molecule, and view electronic and nuclear motion on their intrinsic scales (attoseconds and Ångstroms). These sources have enabled coherent diffractive imaging, where one can image non-crystalline objects in three dimensions on ultrafast timescales, potentially with atomic resolution. The unprecedented intensity available with XFELs has opened new fields of multiphoton and nonlinear x-ray physics where behavior of matter under extreme conditions can be explored. The unprecedented time resolution and pulse synchronization provided by HHG sources has kindled fundamental investigations of time delays in photoionization, charge migration in molecules, and dynamics near conical intersections that are foundational to AMO physics and chemistry. This roadmap coincides with the year when three new XFEL facilities, operating at Ångstrom wavelengths, opened for users (European XFEL, Swiss-FEL and PAL-FEL in Korea) almost doubling the present worldwide number of XFELs, and documents the remarkable progress in HHG capabilities since its discovery roughly 30 years ago, showcasing experiments in AMO physics and other applications. Here we capture the perspectives of 17 leading groups and organize the contributions into four categories: ultrafast molecular dynamics, multidimensional x-ray spectroscopies; high-intensity x-ray phenomena; attosecond x-ray science.
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| 3. |
- Bengtsson, Samuel N., et al.
(författare)
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Free induction decay in the extreme ultraviolet
- 2015
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Ingår i: Proceedings of Frontiers in Optics 2015, FIO 2015. - 9781943580033
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Konferensbidrag (refereegranskat)abstract
- We present an experimental study of controlled Free Induction Decay (FID) in the extreme ultraviolet regime excited by High-order Harmonics. The control is done by applying a delayed infrared pulse.
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| 4. |
- Brizuela, Fernando, et al.
(författare)
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Efficient high order harmonic generation boosted by below threshold harmonics
- 2013
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Ingår i: Scientific Reports. - : Springer Science and Business Media LLC. - 2045-2322. ; 3
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Tidskriftsartikel (refereegranskat)abstract
- High-order harmonic generation (HHG) in gases has been established as an important technique for the generation of coherent extreme ultraviolet (XUV) pulses at ultrashort time scales. Its main drawback, however, is the low conversion efficiency, setting limits for many applications, such as ultrafast coherent imaging, nonlinear processes in the XUV range, or seeded free electron lasers. Here we introduce a novel scheme based on using below-threshold harmonics, generated in a seeding cell, to boost the HHG process in a generation cell, placed further downstream in the focused laser beam. By modifying the fundamental driving field, these low-order harmonics alter the ionization step of the nonlinear HHG process. Our dual-cell scheme enhances the conversion efficiency of HHG, opening the path for the realization of robust intense attosecond XUV sources.
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| 5. |
- 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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| 6. |
- 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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| 7. |
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| 8. |
- 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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| 9. |
- 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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| 10. |
- Jimenez-Galan, A., et al.
(författare)
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Phase Measurement of a Fano Resonance Using Tunable Attosecond Pulses
- 2015
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Ingår i: Journal of Physics: Conference Series. - : IOP Publishing. - 1742-6588 .- 1742-6596. ; 635, s. 092137-092137
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Konferensbidrag (refereegranskat)abstract
- We study photoionization of argon atoms close to the 3s(2)3p(6) -> 3s(1)3p(6)4p Fano resonance using an attosecond pulse train and a weak infrared probe field. An interferometric technique combined with tunable attosecond pulses allows us to determine the phase of the photoionization amplitude as a function of photon energy. We interpret the experimental results using an analytical two-photon model based on the Fano formalism and obtain quantitative agreement.
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| 11. |
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| 12. |
- Kotur, Marija, et al.
(författare)
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Spectral phase measurement of a Fano resonance using tunable attosecond pulses
- 2016
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 7
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Tidskriftsartikel (refereegranskat)abstract
- Electron dynamics induced by resonant absorption of light is of fundamental importance in nature and has been the subject of countless studies in many scientific areas. Above the ionization threshold of atomic or molecular systems, the presence of discrete states leads to autoionization, which is an interference between two quantum paths: direct ionization and excitation of the discrete state coupled to the continuum. Traditionally studied with synchrotron radiation, the probability for autoionization exhibits a universal Fano intensity profile as a function of excitation energy. However, without additional phase information, the full temporal dynamics cannot be recovered. Here we use tunable attosecond pulses combined with weak infrared radiation in an interferometric setup to measure not only the intensity but also the phase variation of the photoionization amplitude across an autoionization resonance in argon. The phase variation can be used as a fingerprint of the interactions between the discrete state and the ionization continua, indicating a new route towards monitoring electron correlations in time.
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| 13. |
- Kroon, David, et al.
(författare)
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Attosecond pulse walk-off in high-order harmonic generation
- 2014
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Ingår i: Optics Letters. - 0146-9592. ; 39:7, s. 2218-2221
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Tidskriftsartikel (refereegranskat)abstract
- We study the influence of the generation conditions on the group delay of attosecond pulses in high-order harmonic generation in gases. The group delay relative to the fundamental field is found to decrease with increasing gas pressure in the generation cell, reflecting a temporal walk-off due to the dispersive properties of the nonlinear medium. This effect is well reproduced using an on-axis phase-matching model of high-order harmonic generation in an absorbing gas. (C) 2014 Optical Society of America
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| 14. |
- Larsen, Esben Witting, et al.
(författare)
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Sub-cycle ionization dynamics revealed by trajectory resolved, elliptically-driven high-order harmonic generation
- 2016
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Ingår i: Scientific Reports. - : Springer Science and Business Media LLC. - 2045-2322. ; 6
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Tidskriftsartikel (refereegranskat)abstract
- The sub-cycle dynamics of electrons driven by strong laser fields is central to the emerging field of attosecond science. We demonstrate how the dynamics can be probed through high-order harmonic generation, where different trajectories leading to the same harmonic order are initiated at different times, thereby probing different field strengths. We find large differences between the trajectories with respect to both their sensitivity to driving field ellipticity and resonant enhancement. To accurately describe the ellipticity dependence of the long trajectory harmonics we must include a sub-cycle change of the initial velocity distribution of the electron and its excursion time. The resonant enhancement is observed only for the long trajectory contribution of a particular harmonic when a window resonance in argon, which is off-resonant in the field-free case, is shifted into resonance due to a large dynamic Stark shift.
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| 15. |
- Litaize, Olivier, et al.
(författare)
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New results in the modeling of fission and radiative neutron capture with FIFRELIN
- 2023
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Ingår i: 15TH INTERNATIONAL CONFERENCE ON NUCLEAR DATA FOR SCIENCE AND TECHNOLOGY, ND2022. - : EDP Sciences.
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Konferensbidrag (refereegranskat)abstract
- The FIFRELIN Monte Carlo code has been upgraded recently by adding new capabilities, additional models and updated databases. Several examples are presented in this work as well as three different applications related to the prompt component in fission, gamma cascades from thermal neutron capture and the delayed component in fission associated to the time evolution of decay heat.
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| 16. |
- Louisy, Maite, et al.
(författare)
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Gating attosecond pulses in a noncollinear geometry
- 2015
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Ingår i: Optica. - 2334-2536. ; 2:6, s. 563-566
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Tidskriftsartikel (refereegranskat)abstract
- The efficient generation of isolated attosecond pulses (IAPs), giving access to ultrafast electron dynamics in various systems, is a key challenge in attosecond science. IAPs can be produced by confining the extreme ultraviolet emission generated by an intense laser pulse to a single field half-cycle or, as shown recently, by employing angular streaking methods. Here, we experimentally demonstrate the angular streaking of attosecond pulse trains in a noncollinear geometry, leading to the emission of angularly separated IAPs. The noncollinear geometry simplifies the separation of the fundamental laser field and the generated pulses, making this scheme promising for intracavity attosecond pulse generation, thus opening new possibilities for high-repetition-rate attosecond sources. (C) 2015 Optical Society of America
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| 17. |
- Månsson, Erik, et al.
(författare)
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Double ionization probed on the attosecond timescale
- 2014
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Ingår i: Nature Physics. - 1745-2473 .- 1745-2481. ; 10:3, s. 207-211
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Tidskriftsartikel (refereegranskat)abstract
- Double ionization following the absorption of a single photon is one of the most fundamental processes requiring interaction between electrons(1-3). Information about this interaction is usually obtained by detecting emitted particles without access to real-time dynamics. Here, attosecond light pulses(4,5), electron wave packet interferometry(6) and coincidence techniques(7) are combined to measure electron emission times in double ionization of xenon using single ionization as a clock, providing unique insight into the two-electron ejection mechanism. Access to many-particle dynamics in real time is of fundamental importance for understanding processes induced by electron correlation in atomic, molecular and more complex systems.
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| 18. |
- Månsson, Erik, et al.
(författare)
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Multi-purpose two- and three-dimensional momentum imaging of charged particles for attosecond experiments at 1 kHz repetition rate.
- 2014
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Ingår i: Review of Scientific Instruments. - : AIP Publishing. - 1089-7623 .- 0034-6748. ; 85:12
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Tidskriftsartikel (refereegranskat)abstract
- We report on the versatile design and operation of a two-sided spectrometer for the imaging of charged-particle momenta in two dimensions (2D) and three dimensions (3D). The benefits of 3D detection are to discern particles of different mass and to study correlations between fragments from multi-ionization processes, while 2D detectors are more efficient for single-ionization applications. Combining these detector types in one instrument allows us to detect positive and negative particles simultaneously and to reduce acquisition times by using the 2D detector at a higher ionization rate when the third dimension is not required. The combined access to electronic and nuclear dynamics available when both sides are used together is important for studying photoreactions in samples of increasing complexity. The possibilities and limitations of 3D momentum imaging of electrons or ions in the same spectrometer geometry are investigated analytically and three different modes of operation demonstrated experimentally, with infrared or extreme ultraviolet light and an atomic/molecular beam.
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| 19. |
- Peschel, Jasper, et al.
(författare)
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Attosecond dynamics of multi-channel single photon ionization
- 2022
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 13:1
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Tidskriftsartikel (refereegranskat)abstract
- Photoionization of atoms and molecules is one of the fastest processes in nature. The understanding of the ultrafast temporal dynamics of this process often requires the characterization of the different angular momentum channels over a broad energy range. Using a two-photon interferometry technique based on extreme ultraviolet and infrared ultrashort pulses, we measure the phase and amplitude of the individual angular momentum channels as a function of kinetic energy in the outer-shell photoionization of neon. This allows us to unravel the influence of channel interference as well as the effect of the short-range, Coulomb and centrifugal potentials, on the dynamics of the photoionization process.
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| 20. |
- Petersson, C. L.M., et al.
(författare)
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Anisotropic photoemission time delays close to a Fano resonance
- 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
- Electron correlation and multielectron effects are fundamental interactions that govern many physical and chemical processes in atomic, molecular and solid state systems. The process of autoionization, induced by resonant excitation of electrons into discrete states present in the spectral continuum of atomic and molecular targets, is mediated by electron correlation. Here we investigate the attosecond photoemission dynamics in argon in the 20-40 eV spectral range, in the vicinity of the 3s(-1)np autoionizing resonances. We present measurements of the differential photoionization cross section and extract energy and angle-dependent atomic time delays with an attosecond interferometric method. With the support of a theoretical model, we are able to attribute a large part of the measured time delay anisotropy to the presence of autoionizing resonances, which not only distort the phase of the emitted photoelectron wave packet but also introduce an angular dependence.
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| 21. |
- Plach, Marius, et al.
(författare)
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Spatial Aberrations in High-Order Harmonic Generation
- 2024
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Ingår i: Ultrafast Science. - 2097-0331. ; 4
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Tidskriftsartikel (refereegranskat)abstract
- We investigate the spatial characteristics of high-order harmonic radiation generated in argon and observe cross-like patterns in the far field. An analytical model describing harmonics from an astigmatic driving beam reveals that these patterns result from the order and generation position-dependent divergence of harmonics. Even small amounts of driving field astigmatism may result in cross-like patterns, coming from the superposition of individual harmonics with spatial profiles elongated in different directions. By correcting the aberrations using a deformable mirror, we show that fine-tuning the driving wavefront is essential for optimal spatial quality of the harmonics.
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| 22. |
- Zhong, Shiyang, et al.
(författare)
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Attosecond electron–spin dynamics in Xe 4d photoionization
- 2020
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723 .- 2041-1723. ; 11:1
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Tidskriftsartikel (refereegranskat)abstract
- The photoionization of xenon atoms in the 70–100 eV range reveals several fascinating physical phenomena such as a giant resonance induced by the dynamic rearrangement of the electron cloud after photon absorption, an anomalous branching ratio between intermediate Xe+ states separated by the spin-orbit interaction and multiple Auger decay processes. These phenomena have been studied in the past, using in particular synchrotron radiation, but without access to real-time dynamics. Here, we study the dynamics of Xe 4d photoionization on its natural time scale combining attosecond interferometry and coincidence spectroscopy. A time-frequency analysis of the involved transitions allows us to identify two interfering ionization mechanisms: the broad giant dipole resonance with a fast decay time less than 50 as, and a narrow resonance at threshold induced by spin-flip transitions, with much longer decay times of several hundred as. Our results provide insight into the complex electron-spin dynamics of photo-induced phenomena.
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