| 1. |
- Barillot, T., et al.
(författare)
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Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule
- 2021
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Ingår i: Physical Review X. - : American Physical Society. - 2160-3308. ; 11:3
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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.
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| 2. |
- Allaria, E., et al.
(författare)
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Highly coherent and stable pulses from the FERMI seeded free-electron laser in the extreme ultraviolet
- 2012
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Ingår i: Nature Photonics. - 1749-4885. ; 6:10, s. 699-704
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Tidskriftsartikel (refereegranskat)abstract
- Free-electron lasers (FELs) are promising devices for generating light with laser-like properties in the extreme ultraviolet and X-ray spectral regions. Recently, FELs based on the self-amplified spontaneous emission (SASE) mechanism have allowed major breakthroughs in diffraction and spectroscopy applications, despite the relatively large shot-to-shot intensity and photon-energy fluctuations and the limited longitudinal coherence inherent in the SASE mechanism. Here, we report results on the initial performance of the FERMI seeded FEL, based on the high-gain harmonic generation configuration, in which an external laser is used to initiate the emission process. Emission from the FERMI FEL-1 source occurs in the form of pulses carrying energy of several tens of microjoules per pulse and tunable throughout the 65 to 20 nm wavelength range, with unprecedented shot-to-shot wavelength stability, low-intensity fluctuations, close to transform-limited bandwidth, transverse and longitudinal coherence and full control of polarization.
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| 3. |
- Sanchez-Gonzalez, A., et al.
(författare)
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Accurate prediction of X-ray pulse properties from a free-electron laser using machine learning
- 2017
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 8
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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.
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| 4. |
- Hartmann, G., et al.
(författare)
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Circular dichroism measurements at an x-ray free-electron laser with polarization control
- 2016
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Ingår i: Review of Scientific Instruments. - : AIP Publishing. - 0034-6748 .- 1089-7623. ; 87:8
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Tidskriftsartikel (refereegranskat)abstract
- A non-destructive diagnostic method for the characterization of circularly polarized, ultraintense, short wavelength free-electron laser (FEL) light is presented. The recently installed Delta undulator at the LCLS (Linac Coherent Light Source) at SLAC National Accelerator Laboratory (USA) was used as showcase for this diagnostic scheme. By applying a combined two-color, multi-photon experiment with polarization control, the degree of circular polarization of the Delta undulator has been determined. Towards this goal, an oriented electronic state in the continuum was created by non-resonant ionization of the O2 1s core shell with circularly polarized FEL pulses at hν 700 eV. An also circularly polarized, highly intense UV laser pulse with hν 3.1 eV was temporally and spatially overlapped, causing the photoelectrons to redistribute into so-called sidebands that are energetically separated by the photon energy of the UV laser. By determining the circular dichroism of these redistributed electrons using angle resolving electron spectroscopy and modeling the results with the strong-field approximation, this scheme allows to unambiguously determine the absolute degree of circular polarization of any pulsed, ultraintense XUV or X-ray laser source. © 2016 Author(s).
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| 5. |
- Hartmann, N., et al.
(författare)
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Attosecond time-energy structure of X-ray free-electron laser pulses
- 2018
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Ingår i: Nature Photonics. - : Springer Science and Business Media LLC. - 1749-4885 .- 1749-4893. ; 12:4, s. 215-220
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Tidskriftsartikel (refereegranskat)abstract
- The time-energy information of ultrashort X-ray free-electron laser pulses generated by the Linac Coherent Light Source is measured with attosecond resolution via angular streaking of neon 1s photoelectrons. The X-ray pulses promote electrons from the neon core level into an ionization continuum, where they are dressed with the electric field of a circularly polarized infrared laser. This induces characteristic modulations of the resulting photoelectron energy and angular distribution. From these modulations we recover the single-shot attosecond intensity structure and chirp of arbitrary X-ray pulses based on self-amplified spontaneous emission, which have eluded direct measurement so far. We characterize individual attosecond pulses, including their instantaneous frequency, and identify double pulses with well-defined delays and spectral properties, thus paving the way for X-ray pump/X-ray probe attosecond free-electron laser science. © 2018 The Author(s).
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| 6. |
- Lutman, A. A., et al.
(författare)
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Polarization control in an X-ray free-electron laser
- 2016
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Ingår i: Nature Photonics. - : Springer Science and Business Media LLC. - 1749-4885 .- 1749-4893. ; 10:7, s. 468-472
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Tidskriftsartikel (refereegranskat)abstract
- X-ray free-electron lasers are unique sources of high-brightness coherent radiation. However, existing devices supply only linearly polarized light, precluding studies of chiral dynamics. A device called the Delta undulator has been installed at the Linac Coherent Light Source (LCLS) to provide tunable polarization. With a reverse tapered planar undulator line to pre-microbunch the beam and the novel technique of beam diverting, hundreds of microjoules of circularly polarized X-ray pulses are produced at 500-1,200 eV. These X-ray pulses are tens of femtoseconds long, have a degree of circular polarization of 0.98(+0.02)(-0.04) at 707 eV and may be scanned in energy. We also present a new two-colour X-ray pump-X-ray probe operating mode for the LCLS. Energy differences of Delta E/E = 2.4% are supported, and the second pulse can be adjusted to any elliptical polarization. In this mode, the pointing, timing, intensity and wavelength of the two pulses can be modified.
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| 7. |
- Heider, R., et al.
(författare)
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Megahertz-compatible angular streaking with few-femtosecond resolution at x-ray free-electron lasers
- 2019
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Ingår i: Physical Review A. - 2469-9926. ; 100:5
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Tidskriftsartikel (refereegranskat)abstract
- Highly brilliant, coherent, femtosecond x-ray pulses delivered by free-electron lasers (FELs) constitute one of the pillars of modern ultrafast science. Next generation FEL facilities provide up to megahertz repetition rates and pulse durations down to the attosecond regime utilizing self-amplification of spontaneous emission. However, the stochastic nature of this generation mechanism demands single-shot pulse characterization to perform meaningful experiments. Here we demonstrate a fast yet robust online analysis technique capable of megahertz-rate mapping of the temporal intensity structure and arrival time of x-ray FEL pulses with few-femtosecond resolution. We performed angular streaking measurements of both neon photo- and Auger electrons and show their applicability for a direct time-domain feedback system during ongoing experiments. The fidelity of the real-time pulse characterization algorithm is corroborated by resolving isolated x-ray pulses and double pulse trains with few-femtosecond substructure, thus paving the way for x-ray-pump-x-ray-probe FEL science at repetition rates compatible with the demands of LCLS-II and European XFEL.
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| 8. |
- Li, S., et al.
(författare)
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Two-dimensional correlation analysis for x-ray photoelectron spectroscopy
- 2021
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Ingår i: Journal of Physics B. - : Institute of Physics Publishing (IOPP). - 0953-4075 .- 1361-6455. ; 54:14
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Tidskriftsartikel (refereegranskat)abstract
- X-ray photoelectron spectroscopy (XPS) measures the binding energy of core-level electrons, which are well-localised to specific atomic sites in a molecular system, providing valuable information on the local chemical environment. The technique relies on measuring the photoelectron spectrum upon x-ray photoionisation, and the resolution is often limited by the bandwidth of the ionising x-ray pulse. This is particularly problematic for time-resolved XPS, where the desired time resolution enforces a fundamental lower limit on the bandwidth of the x-ray source. In this work, we report a novel correlation analysis which exploits the correlation between the x-ray and photoelectron spectra to improve the resolution of XPS measurements. We show that with this correlation-based spectral-domain ghost imaging method we can achieve sub-bandwidth resolution in XPS measurements. This analysis method enables XPS for sources with large bandwidth or spectral jitter, previously considered unfeasible for XPS measurements.
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| 9. |
- Akeroyd, Michael A., et al.
(författare)
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International Collegium of Rehabilitative Audiology (ICRA) recommendations for the construction of multilingual speech tests ICRA Working Group on Multilingual Speech Tests
- 2015
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Ingår i: International Journal of Audiology. - : TAYLOR & FRANCIS LTD. - 1499-2027 .- 1708-8186. ; 54, s. 17-22
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Tidskriftsartikel (refereegranskat)abstract
- Objective: To provide guidelines for the development of two types of closed-set speech-perception tests that can be applied and interpreted in the same way across languages. The guidelines cover the digit triplet and the matrix sentence tests that are most commonly used to test speech recognition in noise. They were developed by a working group on Multilingual Speech Tests of the International Collegium of Rehabilitative Audiology (ICRA). Design: The recommendations are based on reviews of existing evaluations of the digit triplet and matrix tests as well as on the research experience of members of the ICRA Working Group. They represent the results of a consensus process. Results: The resulting recommendations deal with: Test design and word selection; Talker characteristics; Audio recording and stimulus preparation; Masking noise; Test administration; and Test validation. Conclusions: By following these guidelines for the development of any new test of this kind, clinicians and researchers working in any language will be able to perform tests whose results can be compared and combined in cross-language studies.
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| 10. |
- Assefa, T. A., et al.
(författare)
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The fluctuation–dissipation measurement instrument at the Linac Coherent Light Source
- 2022
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Ingår i: Review of Scientific Instruments. - : AIP Publishing. - 1089-7623 .- 0034-6748. ; 93
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Tidskriftsartikel (refereegranskat)abstract
- The development of new modes at x-ray free electron lasers has inspired novel methods for studying fluctuations at different energies and timescales. For closely spaced x-ray pulses that can be varied on ultrafast time scales, we have constructed a pair of advanced instruments to conduct studies targeting quantum materials. We first describe a prototype instrument built to test the proof-of-principle of resonant magnetic scattering using ultrafast pulse pairs. This is followed by a description of a new endstation, the so-called fluctuation–dissipation measurement instrument, which was used to carry out studies with a fast area detector. In addition, we describe various types of diagnostics for single-shot contrast measurements, which can be used to normalize data on a pulse-by-pulse basis and calibrate pulse amplitude ratios, both of which are important for the study of fluctuations in materials. Furthermore, we present some new results using the instrument that demonstrates access to higher momentum resolution.
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| 11. |
- 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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| 12. |
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| 13. |
- Maroju, P. K., et al.
(författare)
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Analysis of two-color photoelectron spectroscopy for attosecond metrology at seeded free-electron lasers
- 2021
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Ingår i: New Journal of Physics. - : IOP Publishing. - 1367-2630. ; 23:4
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Tidskriftsartikel (refereegranskat)abstract
- The generation of attosecond pulse trains at free-electron lasers opens new opportunities in ultrafast science, as it gives access, for the first time, to reproducible, programmable, extreme ultraviolet (XUV) waveforms with high intensity. In this work, we present a detailed analysis of the theoretical model underlying the temporal characterization of the attosecond pulse trains recently generated at the free-electron laser FERMI. In particular, the validity of the approximations used for the correlated analysis of the photoelectron spectra generated in the two-color photoionization experiments are thoroughly discussed. The ranges of validity of the assumptions, in connection with the main experimental parameters, are derived.
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| 14. |
- Rohringer, N., et al.
(författare)
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Stimulated X-Ray Raman Scattering with Free-Electron Laser Sources
- 2016
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Ingår i: X-Ray Lasers 2014. - Cham : Springer. - 0930-8989. - 9783319195216 - 9783319195209 ; , s. 201-207
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Bokkapitel (refereegranskat)abstract
- Stimulated electronic x-ray Raman scattering is the building block for several proposed x-ray pump probe techniques, that would allow the study of electron dynamics at unprecedented timescales.We present high spectral resolution data on stimulated electronic x-ray Raman scattering in a gas sample of neon using a self-amplified spontaneous emission x-ray free-electron laser. Despite the limited spectral coherence and broad bandwidth of these sources, high-resolution spectra can be obtained by statistical methods, opening the path to coherent stimulated x-ray Raman spectroscopy. An extension of these ideas to molecules and the results of a recent experiment in CO are discussed.
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| 15. |
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| 16. |
- Dreschler, W. A., et al.
(författare)
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Charactering the individual ear by the "Auditory Profile
- 2008
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Ingår i: Journal of the Acoustical Society of America. - Melville, NY, USA : A I P Publishing LLC. - 0001-4966 .- 1520-8524. ; 123:5
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Tidskriftsartikel (refereegranskat)abstract
- This paper describes a new approach to auditory diagnostics, which is one of the central themes of the EU-project HEARCOM. For this purpose we defined a so-called "Auditory Profile" that can be assessed for each individual listener using a standardized battery of audiological tests that - in addition to the pure-tone audiogram - focus on loudness perception, frequency resolution, temporal acuity, speech perception, binaural functioning, listening effort, subjective hearing abilities, and cognition. For the sake of testing time only summary tests are included from each of these areas, but the broad approach of characterizing auditory communication problems by means of standardized test is expected to have an added value above traditional testing in understanding the reasons for poor speech reception. The Auditory profile may also be relevant in the field of auditory rehabilitation and for design of acoustical environments. The results of an international 5-center study (in 4 countries and in 4 languages) will be presented and the relevance of a broad but well-standardized approach will be discussed.
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| 17. |
- Dreschler, W. A., et al.
(författare)
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D-2-6: Report about the results of the multicentre evaluation of the Auditory Profile. Public report
- 2009
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Rapport (övrigt vetenskapligt/konstnärligt)abstract
- Twenty-eight partners participated in the FP6 EU-funded project HearCom, with the goal to improve hearing in our communication society. One of the main achievements has been the provision of advanced hearing screening tests by telephone and Internet. For hearing diagnostics it was aimed at the harmonization of hearing diagnostic tests within Europe. For this the concept of the Auditory Profile has been developed with several tests for various languages. Hearing problems are also a result of adverse acoustical circumstances for which the effects have been studied, modelled and evaluated for hearing impaired. For hearing rehabilitation a large scale comparison study was performed on signal enhancement techniques (algorithms) for hearing devices. Modern technology may assist on hearing and communication by the use of wireless technology and automatic speech transcription. On this it is shown that improvements for auditory communication can be obtained, but that technology should develop further. An overview is given on the HearCom portal with sections for screening diagnostics, hearing information for the public and professionals, and a new service called HearCompanion that provides step-by-step support for the hearing rehabilitation process.
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| 18. |
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| 19. |
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| 20. |
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| 21. |
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| 22. |
- Higley, Daniel J., et al.
(författare)
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Femtosecond X-ray induced changes of the electronic and magnetic response of solids from electron redistribution
- 2019
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Ingår i: Nature Communications. - : Nature Publishing Group. - 2041-1723. ; 10
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Tidskriftsartikel (refereegranskat)abstract
- Resonant X-ray absorption, where an X-ray photon excites a core electron into an unoccupied valence state, is an essential process in many standard X-ray spectroscopies. With increasing X-ray intensity, the X-ray absorption strength is expected to become nonlinear. Here, we report the onset of such a nonlinearity in the resonant X-ray absorption of magnetic Co/Pd multilayers near the Co L-3 edge. The nonlinearity is directly observed through the change of the absorption spectrum, which is modified in less than 40 fs within 2 eV of its threshold. This is interpreted as a redistribution of valence electrons near the Fermi level. For our magnetic sample this also involves mixing of majority and minority spins, due to sample demagnetization. Our findings reveal that nonlinear X-ray responses of materials may already occur at relatively low intensities, where the macroscopic sample is not destroyed, providing insight into ultrafast charge and spin dynamics.
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| 23. |
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| 24. |
- Kumar Maroju, Praveen, et al.
(författare)
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Attosecond pulse shaping using a seeded free-electron laser
- 2020
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Ingår i: Nature. - : Springer Science and Business Media LLC. - 0028-0836 .- 1476-4687. ; 578, s. 386-391
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Tidskriftsartikel (refereegranskat)abstract
- Attosecond pulses are central to the investigation of valence- and core-electron dynamics on their natural timescales. The reproducible generation and characterization of attosecond waveforms has been demonstrated so far only through the process of high-order harmonic generation. Several methods for shaping attosecond waveforms have been proposed, including the use of metallic filters, multilayer mirrors and manipulation of the driving field. However, none of these approaches allows the flexible manipulation of the temporal characteristics of the attosecond waveforms, and they suffer from the low conversion efficiency of the high-order harmonic generation process. Free-electron lasers, by contrast, deliver femtosecond, extreme-ultraviolet and X-ray pulses with energies ranging from tens of microjoules to a few millijoules. Recent experiments have shown that they can generate subfemtosecond spikes, but with temporal characteristics that change shot-to-shot. Here we report reproducible generation of high-energy (microjoule level) attosecond waveforms using a seeded free-electron laser. We demonstrate amplitude and phase manipulation of the harmonic components of an attosecond pulse train in combination with an approach for its temporal reconstruction. The results presented here open the way to performing attosecond time-resolved experiments with free-electron lasers.
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| 25. |
- Le Guyader, Loïc, et al.
(författare)
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State-resolved ultrafast charge and spin dynamics in [Co/Pd] multilayers
- 2022
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Ingår i: Applied Physics Letters. - : AIP Publishing. - 0003-6951 .- 1077-3118. ; 120:3
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Tidskriftsartikel (refereegranskat)abstract
- We use transient absorption spectroscopy with circularly polarized x rays to detect laser-excited hole states below the Fermi level and compare their dynamics with that of unoccupied states above the Fermi level in ferromagnetic [Co/Pd] multilayers. While below the Fermi level, an instantaneous and significantly stronger demagnetization is observed, above the Fermi level, the demagnetization is delayed by 35 ± 10 fs. This provides a direct visualization of how ultrafast demagnetization proceeds via initial spin-flip scattering of laser-excited holes to the subsequent formation of spin waves.
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