| 1. |
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| 2. |
- Biedron, Sandra, et al.
(författare)
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Workshop on high-harmonic seeding for present and future short wavelength free-electron lasers
- 2009
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Ingår i: Synchrotron Radiation News. - : Informa UK Limited. - 0894-0886 .- 1931-7344. ; 22:4, s. 5-9
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Tidskriftsartikel (refereegranskat)abstract
- We are now seeing the development of a new generation of synchrotron radiation sources, the seeded, short-wavelength Free Electron Lasers (FELs), which are capable of driving the radiation to even higher intensities, and with new capabilities such as longitudinal coherence and ultra-short pulses. The Workshop on High-harmonic Seeding for Present and Future Short Wavelength Free-Electron Lasers, hosted by Sincrotrone Trieste, ENEA, INFN-LNF, and the University of Rome, dealt with the initial stage of creating such intense beams, namely the seeding necessary for initiating the lasing process. More than 50 participants from all over the world met on December 3–5, 2008, at the INFN/LNF at Frascati (Italy) to discuss high-harmonic seeding of FELs and was stimulated by a previous and more general meeting held in Lund (Sweden) in 2007 [1].
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| 3. |
- Diesen, Elias, et al.
(författare)
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Ultrafast Adsorbate Excitation Probed with Subpicosecond-Resolution X-Ray Absorption Spectroscopy
- 2021
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Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 127:1
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Tidskriftsartikel (refereegranskat)abstract
- We use a pump-probe scheme to measure the time evolution of the C K-edge x-ray absorption spectrum from CO/Ru(0001) after excitation by an ultrashort high-intensity optical laser pulse. Because of the short duration of the x-ray probe pulse and precise control of the pulse delay, the excitation-induced dynamics during the first picosecond after the pump can be resolved with unprecedented time resolution. By comparing with density functional theory spectrum calculations, we find high excitation of the internal stretch and frustrated rotation modes occurring within 200 fs of laser excitation, as well as thermalization of the system in the picosecond regime. The ∼100 fs initial excitation of these CO vibrational modes is not readily rationalized by traditional theories of nonadiabatic coupling of adsorbates to metal surfaces, e.g., electronic frictions based on first order electron-phonon coupling or transient population of adsorbate resonances. We suggest that coupling of the adsorbate to nonthermalized electron-hole pairs is responsible for the ultrafast initial excitation of the modes.
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| 4. |
- Fushitani, Mizuho, et al.
(författare)
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Time-resolved photoelectron imaging of complex resonances in molecular nitrogen
- 2021
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Ingår i: The Journal of chemical physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 154:14
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Tidskriftsartikel (refereegranskat)abstract
- We have used the FERMI free-electron laser to perform time-resolved photoelectron imaging experiments on a complex group of resonances near 15.38 eV in the absorption spectrum of molecular nitrogen, N2, under jet-cooled conditions. The new data complement and extend the earlier work of Fushitani et al. [Opt. Express 27, 19702–19711 (2019)], who recorded time-resolved photoelectron spectra for this same group of resonances. Time-dependent oscillations are observed in both the photoelectron yields and the photoelectron angular distributions, providing insight into the interactions among the resonant intermediate states. In addition, for most states, we observe an exponential decay of the photoelectron yield that depends on the ionic final state. This observation can be rationalized by the different lifetimes for the intermediate states contributing to a particular ionization channel. Although there are nine resonances within the group, we show that by detecting individual photoelectron final states and their angular dependence, we can identify and differentiate quantum pathways within this complex system.
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| 5. |
- Fushitani, Mizuho, et al.
(författare)
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Wave packet dynamics and control in excited states of molecular nitrogen
- 2024
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Ingår i: The Journal of chemical physics. - 0021-9606. ; 160:10
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Tidskriftsartikel (refereegranskat)abstract
- Wave packet interferometry with vacuum ultraviolet light has been used to probe a complex region of the electronic spectrum of molecular nitrogen, N2. Wave packets of Rydberg and valence states were excited by using double pulses of vacuum ultraviolet (VUV), free-electron-laser (FEL) light. These wave packets were composed of contributions from multiple electronic states with a moderate principal quantum number (n ∼ 4-9) and a range of vibrational and rotational quantum numbers. The phase relationship of the two FEL pulses varied in time, but as demonstrated previously, a shot-by-shot analysis allows the spectra to be sorted according to the phase between the two pulses. The wave packets were probed by angle-resolved photoionization using an infrared pulse with a variable delay after the pair of excitation pulses. The photoelectron branching fractions and angular distributions display oscillations that depend on both the time delays and the relative phases of the VUV pulses. The combination of frequency, time delay, and phase selection provides significant control over the ionization process and ultimately improves the ability to analyze and assign complex molecular spectra.
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| 6. |
- Khan, Shaukat, et al.
(författare)
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Evolution of density-modulated electron beams in drift sections
- 2024
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Ingår i: Physical Review Accelerators and Beams. - : American Physical Society. - 2469-9888. ; 27:4
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Tidskriftsartikel (refereegranskat)abstract
- Initiating the amplification process in a short-wavelength free-electron laser (FEL) by external seed laser pulses results in radiation with a high degree of longitudinal and transverse coherence. The basic layout in seeded harmonic generation involves a periodic electron energy modulation by laser-electron interaction in a short undulator (the "modulator"), which is converted into a density modulation in a dispersive section immediately followed by a long FEL undulator (the "radiator") tuned to a harmonic of the seed laser wavelength. With the advent of more complex seeding schemes, density-modulated beams may need to be transported in drift sections before entering the radiator. Long FEL undulators may also contain several drift spaces to accommodate focusing elements and diagnostics. Therefore, it is of general interest to study the evolution of density-modulated electron beams in drift sections under the influence of repulsive Coulomb forces. At FERMI, a seeded FEL user facility in Trieste, Italy, systematic studies of the impact of varying drift length on coherent harmonic emission were undertaken. In order to make the underlying physics transparent, the emphasis of this paper is on reproducing the experimental findings with analytical estimates and a simple one-dimensional numerical model. Furthermore, the Coulomb forces in a drift section may be employed to enhance the laser-induced energy modulation and yield an improved density modulation before entering the FEL radiator.
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| 7. |
- 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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| 8. |
- LaRue, Jerry, et al.
(författare)
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Symmetry-resolved CO desorption and oxidation dynamics on O/Ru(0001) probed at the C K-edge by ultrafast x-ray spectroscopy
- 2022
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 157:16
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Tidskriftsartikel (refereegranskat)abstract
- We report on carbon monoxide desorption and oxidation induced by 400 nm femtosecond laser excitation on the O/Ru(0001) surface probed by time-resolved x-ray absorption spectroscopy (TR-XAS) at the carbon K-edge. The experiments were performed under constant background pressures of CO (6 × 10−8 Torr) and O2 (3 × 10−8 Torr). Under these conditions, we detect two transient CO species with narrow 2π* peaks, suggesting little 2π* interaction with the surface. Based on polarization measurements, we find that these two species have opposing orientations: (1) CO favoring a more perpendicular orientation and (2) CO favoring a more parallel orientation with respect to the surface. We also directly detect gas-phase CO2 using a mass spectrometer and observe weak signatures of bent adsorbed CO2 at slightly higher x-ray energies than the 2π* region. These results are compared to previously reported TR-XAS results at the O K-edge, where the CO background pressure was three times lower (2 × 10−8 Torr) while maintaining the same O2 pressure. At the lower CO pressure, in the CO 2π* region, we observed adsorbed CO and a distribution of OC–O bond lengths close to the CO oxidation transition state, with little indication of gas-like CO. The shift toward “gas-like” CO species may be explained by the higher CO exposure, which blocks O adsorption, decreasing O coverage and increasing CO coverage. These effects decrease the CO desorption barrier through dipole–dipole interaction while simultaneously increasing the CO oxidation barrier.
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| 9. |
- Maroju, Praveen K., et al.
(författare)
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A Novel Attosecond Timing Tool for Free-Electron Laser Experiment
- 2020
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Ingår i: High Intensity Lasers and High Field Phenomena 2020. - 9781943580736
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Konferensbidrag (refereegranskat)abstract
- We demonstrate a novel timing tool for Free-Electron Lasers to determine the delay between an attosecond pulse train and infrared pulse with sub-optical-cycle resolu-. tion.
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| 10. |
- Maroju, Praveen Kumar, et al.
(författare)
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Complex attosecond waveform synthesis at fel fermi
- 2021
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Ingår i: Applied Sciences (Switzerland). - : MDPI AG. - 2076-3417. ; 11:21
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Tidskriftsartikel (refereegranskat)abstract
- Free-electron lasers (FELs) can produce radiation in the short wavelength range extending from the extreme ultraviolet (XUV) to the X-rays with a few to a few tens of femtoseconds pulse duration. These facilities have enabled significant breakthroughs in the field of atomic, molecular, and optical physics, implementing different schemes based on two-color photoionization mechanisms. In this article, we present the generation of attosecond pulse trains (APTs) at the seeded FEL FERMI using the beating of multiple phase-locked harmonics. We demonstrate the complex attosecond waveform shaping of the generated APTs, exploiting the ability to manipulate independently the amplitudes and the phases of the harmonics. The described generalized attosecond waveform synthesis technique with an arbitrary number of phase-locked harmonics will allow the generation of sub-100 as pulses with programmable electric fields.
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| 11. |
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| 12. |
- Nandi, Saikat, et al.
(författare)
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Generation of entanglement using a short-wavelength seeded free-electron laser
- 2024
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Ingår i: SCIENCE ADVANCES. - 2375-2548. ; 10:16
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Tidskriftsartikel (refereegranskat)abstract
- Quantum entanglement between the degrees of freedom encountered in the classical world is challenging to observe due to the surrounding environment. To elucidate this issue, we investigate the entanglement generated over ultrafast timescales in a bipartite quantum system comprising two massive particles: a free-moving photoelectron, which expands to a mesoscopic length scale, and a light-dressed atomic ion, which represents a hybrid state of light and matter. Although the photoelectron spectra are measured classically, the entanglement allows us to reveal information about the dressed-state dynamics of the ion and the femtosecond extreme ultraviolet pulses delivered by a seeded free-electron laser. The observed generation of entanglement is interpreted using the time-dependent von Neumann entropy. Our results unveil the potential for using short-wavelength coherent light pulses from free-electron lasers to generate entangled photoelectron and ion systems for studying spooky action at a distance.
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| 13. |
- Nandi, Saikat, et al.
(författare)
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Unraveling Rabi dynamics with a seeded FEL at XUV wavelength
- 2023
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Ingår i: 2023 Conference on Lasers and Electro-Optics Europe and European Quantum Electronics Conference, CLEO/Europe-EQEC 2023. - 9798350345995
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Konferensbidrag (refereegranskat)abstract
- Rabi oscillations, a prominent feature of coherent light-matter interaction arise when a two-level system interacts periodically with an external electromagnetic field [1]. Despite being a cornerstone in quantum physics, they are usually studied in the long-wavelength region, ranging from mid-infrared to visible. Here, we demonstrate that intense femtosecond extreme-ultraviolet (XUV) pulses from FERMI seeded free-electron laser [2] can drive Rabi oscillations between the two levels: 1s2 and 1s4p in helium.
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| 14. |
- Wang, Hsin-Yi, et al.
(författare)
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Time-resolved observation of transient precursor state of CO on Ru(0001) using carbon K-edge spectroscopy
- 2020
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Ingår i: Physical Chemistry, Chemical Physics - PCCP. - 1463-9076 .- 1463-9084. ; 22:5, s. 2677-2684
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Tidskriftsartikel (refereegranskat)abstract
- The transient dynamics of carbon monoxide (CO) molecules on a Ru(0001) surface following femtosecond optical laser pump excitation has been studied by monitoring changes in the unoccupied electronic structure using an ultrafast X-ray free-electron laser (FEL) probe. The particular symmetry of perpendicularly chemisorbed CO on the surface is exploited to investigate how the molecular orientation changes with time by varying the polarization of the FEL pulses. The time evolution of spectral features corresponding to the desorption precursor state was well distinguished due to the narrow line-width of the C K-edge in the X-ray absorption (XA) spectrum, illustrating that CO molecules in the precursor state rotated freely and resided on the surface for several picoseconds. Most of the CO molecules trapped in the precursor state ultimately cooled back down to the chemisorbed state, while we estimate that ∼14.5 ± 4.9% of the molecules in the precursor state desorbed into the gas phase. It was also observed that chemisorbed CO molecules diffused over the metal surface from on-top sites toward highly coordinated sites. In addition, a new “vibrationally hot precursor” state was identified in the polarization-dependent XA spectra.
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| 15. |
- Wituschek, Andreas, et al.
(författare)
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High-gain harmonic generation with temporally overlapping seed pulses and application to ultrafast spectroscopy
- 2020
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Ingår i: Optics Express. - 1094-4087. ; 28, s. 29976-90
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Tidskriftsartikel (refereegranskat)abstract
- Collinear double-pulse seeding of the High-Gain Harmonic Generation (HGHG) process in a free-electron laser (FEL) is a promising approach to facilitate various coherent nonlinear spectroscopy schemes in the extreme ultraviolet (XUV) spectral range. However, in collinear arrangements using a single nonlinear medium, temporally overlapping seed pulses may introduce nonlinear mixing signals that compromise the experiment at short time delays. Here, we investigate these effects in detail by extending the analysis described in a recent publication (Wituschek et al., Nat. Commun., 11, 883, 2020). High-order fringe-resolved autocorrelation and wave packet interferometry experiments at photon energies > 23 eV are performed, accompanied by numerical simulations. It turns out that both the autocorrelation and the wave-packet interferometry data are very sensitive to saturation effects and can thus be used to characterize saturation in the HGHG process. Our results further imply that time-resolved spectroscopy experiments are feasible even for time delays smaller than the seed pulse duration.
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| 16. |
- Wituschek, Andreas, et al.
(författare)
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Tracking attosecond electronic coherences using phase-manipulated extreme ultraviolet pulses
- 2020
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 11
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Tidskriftsartikel (refereegranskat)abstract
- The recent development of ultrafast extreme ultraviolet (XUV) coherent light sources bears great potential for a better understanding of the structure and dynamics of matter. Promising routes are advanced coherent control and nonlinear spectroscopy schemes in the XUV energy range, yielding unprecedented spatial and temporal resolution. However, their implementation has been hampered by the experimental challenge of generating XUV pulse sequences with precisely controlled timing and phase properties. In particular, direct control and manipulation of the phase of individual pulses within an XUV pulse sequence opens exciting possibilities for coherent control and multidimensional spectroscopy, but has not been accomplished. Here, we overcome these constraints in a highly time-stabilized and phase-modulated XUV-pump, XUV-probe experiment, which directly probes the evolution and dephasing of an inner subshell electronic coherence. This approach, avoiding any XUV optics for direct pulse manipulation, opens up extensive applications of advanced nonlinear optics and spectroscopy at XUV wavelengths.
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