| 1. |
- Bouaniche, Alexandre, et al.
(författare)
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Vitiated High Karlovitz n-decane/air Turbulent Flames : Scaling Laws and Micro-mixing Modeling Analysis
- 2019
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Ingår i: Flow Turbulence and Combustion. - : SPRINGER. - 1386-6184 .- 1573-1987. ; 102:1, s. 235-252
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Tidskriftsartikel (refereegranskat)abstract
- Turbulent flames with high Karlovitz numbers have deserved further attention in the most recent literature. For a fixed value of the Damkohler number (ratio between an integral mechanical time and a chemical time), the increase of the Karlovitz number (ratio between a chemical time and a micro-mixing time) by an order of magnitude implies the increase of the turbulent Reynolds number by two orders of magnitude (Bray, Symp. (Int.) Combust. 26, 1-26 1996). In the practice of real burners featuring a limited range of variation of their turbulent Reynolds number, high Karlovitz combustion actually goes with a drastic reduction of the Damkohler number. Within this context, the relation between the dilution by burnt gases and the apparition of high Karlovitz flames is discussed. Basic scaling laws are reported which suggest that the overall decrease of the burning rate due to very fast mixing can indeed be compensated by the energy brought to the reaction zone by burnt gases. To estimate the validity of these scaling laws, in particular the response of the quenching Karlovitz versus the dilution level with a vitiated stream, the micro-mixing rate is varied in a multiple-inlet canonical turbulent and reactive micro-mixing problem. A reduced n-decane/air chemical kinetics is used, which has been derived from a more detailed scheme using a combination of a directed relation graphs analysis with a Genetic Algorithm. The multiple-inlet canonical micro-mixing problem includes liquid fuel injection and dilution by burnt gases, both calibrated from conditions representative of an aeronautical combustion chamber. The results confirm the possibility of reaching, with the help of a vitiated mixture, very high Karlovitz combustion before quenching occurs.
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| 2. |
- Burgos Parra, Erick Omar, et al.
(författare)
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Holographic imaging of magnetization in a single layer nano-contact spin transfer oscillator
- 2016
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Ingår i: IEEE transactions on magnetics. - 0018-9464. ; 52:7
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Tidskriftsartikel (refereegranskat)abstract
- Time-averaged images of the magnetization within single layer spin transfer oscillators have been obtained using the holography with extended reference by autocorrelation linear differential operator (HERALDO) technique. Transport measurements on a Pd(5)-Cu(20)-Ni81Fe19(7)-Cu(2)-Pd(2) (in nm) stack with a 100 nm diameter nano-contact reveal the presence of vortex dynamics. Magnetic images of the device for injected current values of 24mA and -24mA suggest that a vortex has been ejected from the nano-contact and become pinned at the edge of the region that is visible through the Au mask.
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| 3. |
- Buzzi, Michele, et al.
(författare)
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Single-shot Monitoring of Ultrafast Processes via X-ray Streaking at a Free Electron Laser
- 2017
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Ingår i: Scientific Reports. - : Nature Publishing Group. - 2045-2322. ; 7
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Tidskriftsartikel (refereegranskat)abstract
- The advent of x-ray free electron lasers has extended the unique capabilities of resonant x-ray spectroscopy techniques to ultrafast time scales. Here, we report on a novel experimental method that allows retrieving with a single x-ray pulse the time evolution of an ultrafast process, not only at a few discrete time delays, but continuously over an extended time window. We used a single x-ray pulse to resolve the laser-induced ultrafast demagnetisation dynamics in a thin cobalt film over a time window of about 1.6 ps with an excellent signal to noise ratio. From one representative single shot measurement we extract a spin relaxation time of (130 +/- 30) fs with an average value, based on 193 single shot events of (113 +/- 20) fs. These results are limited by the achieved experimental time resolution of 120 fs, and both values are in excellent agreement with previous results and theoretical modelling. More generally, this new experimental approach to ultrafast x-ray spectroscopy paves the way to the study of non-repetitive processes that cannot be investigated using traditional repetitive pump-probe schemes.
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| 4. |
- Couto, Rafael C., et al.
(författare)
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Anomalously strong two-electron one-photon X-ray decay transitions in CO caused by avoided crossing
- 2016
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Ingår i: Scientific Reports. - : Nature Publishing Group. - 2045-2322. ; 6
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Tidskriftsartikel (refereegranskat)abstract
- The unique opportunity to study and control electron-nuclear quantum dynamics in coupled potentials offered by the resonant inelastic X-ray scattering (RIXS) technique is utilized to unravel an anomalously strong two-electron one-photon transition from core-excited to Rydberg final states in the CO molecule. High-resolution RIXS measurements of CO in the energy region of 12-14 eV are presented and analyzed by means of quantum simulations using the wave packet propagation formalism and ab initio calculations of potential energy curves and transition dipole moments. The very good overall agreement between the experimental results and the theoretical predictions allows an in-depth interpretation of the salient spectral features in terms of Coulomb mixing of "dark" with "bright" final states leading to an effective two-electron one-photon transition. The present work illustrates that the improved spectral resolution of RIXS spectra achievable today may call for more advanced theories than what has been used in the past.
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| 5. |
- Couto, Rafael C., et al.
(författare)
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Coupled electron-nuclear dynamics in resonant 1 sigma -> 2 pi x-ray Raman scattering of CO molecules
- 2016
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Ingår i: Physical Review A. - : American Physical Society. - 2469-9926. ; 93:3
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Tidskriftsartikel (refereegranskat)abstract
- We present a detailed experimental-theoretical analysis of O K-edge resonant 1 sigma-2 pi inelastic x-ray scattering (RIXS) from carbon monoxide with unprecedented energy resolution. We employ high-level ab initio calculations to compute the potential energy curves of the states involved in the RIXS process and simulate the measured RIXS spectra using the wave-packet-propagation formalism, including Coulomb coupling in the final-state manifold. The theoretical analysis allows us to explain all the key features of the experimental spectra, including some that were not seen before. First, we clearly show the interference effect between different RIXS channels corresponding to the transition via orthogonal (1)Pi(x) and (1)Pi(y) core-excited states of CO. Second, the RIXS region of 13 eV energy loss presents a triple structure, revealed only by the high-resolution measurement. In previous studies, this region was attributed solely to a valence state. Here we show a strong Coulomb mixing of the Rydberg and valence final states, which opens the forbidden RIXS channels to the "dark" final Rydberg states and drastically changes the RIXS profile. Third, using a combination of high-resolution experiment and high-level theory, we improve the vertical bar 4 sigma(-1)2 pi(1)> final-state potential-energy curve by fitting its bottom part with the experiment. Also, the coupling constants between Rydberg and valence states were refined via comparison with the experiment. Our results illustrate the large potential of the RIXS technique for advanced studies of highly excited states of neutral molecules.
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| 6. |
- Couto, Rafael C., et al.
(författare)
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Coupled electron-nuclear dynamics in resonant 1σ→2π x-ray Raman scattering of CO molecules
- 2016
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Ingår i: Physical Review A (Atomic, Molecular and Optical Physics). - 1050-2947. ; 93:3
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Tidskriftsartikel (refereegranskat)abstract
- We present a detailed experimental-theoretical analysis of O K-edge resonant 1σ-2π inelastic x-ray scattering (RIXS) from carbon monoxide with unprecedented energy resolution. We employ high-level ab initio calculations to compute the potential energy curves of the states involved in the RIXS process and simulate the measured RIXS spectra using the wave-packet-propagation formalism, including Coulomb coupling in the final-state manifold. The theoretical analysis allows us to explain all the key features of the experimental spectra, including some that were not seen before. First, we clearly show the interference effect between different RIXS channels corresponding to the transition via orthogonal Πx1 and Πy1 core-excited states of CO. Second, the RIXS region of 13 eV energy loss presents a triple structure, revealed only by the high-resolution measurement. In previous studies, this region was attributed solely to a valence state. Here we show a strong Coulomb mixing of the Rydberg and valence final states, which opens the forbidden RIXS channels to the "dark" final Rydberg states and drastically changes the RIXS profile. Third, using a combination of high-resolution experiment and high-level theory, we improve the |4σ-12π1) final-state potential-energy curve by fitting its bottom part with the experiment. Also, the coupling constants between Rydberg and valence states were refined via comparison with the experiment. Our results illustrate the large potential of the RIXS technique for advanced studies of highly excited states of neutral molecules.
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| 7. |
- Desjardins, Kewin, et al.
(författare)
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Characterization of a back-illuminated CMOS camera for soft x-ray coherent scattering
- 2019
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Ingår i: Proceedings of the 13th International Conference on Synchrotron Radiation Instrumentation, SRI 2018. - : Author(s). - 9780735417823 ; 2054
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Konferensbidrag (refereegranskat)abstract
- A commercial scientific camera has been adapted and characterized at the SOLEIL Synchrotron with the aim to improve the acquisition capabilities on the soft X-ray coherent scattering experimental station at SEXTANTS beamline. This device is equipped by the last generation of back side illuminated scientific CMOS (BSI-sCMOS) of 2048 by 2048 pixels of 11 μm2 able to acquire low noise images with a frame rate up to 48 Hz. The camera's performance measurements have been done and shows a good level of readout noise, a large full-well capacity, a medium dark current and a good homogeneity, respectively, 1.6 e- rms (in High Gain mode), 80 000 e- (in Low Gain mode),<5 e-/pixel/s and ∼ 1%. The quantum efficiency (QE) measurement has been performed at the soft x-ray branch of the METROLOGIE beamline and gives a relatively good agreement with the expected theoretical values. Finally, the demonstration of the camera's efficiency and of the gain in useful time measurement related to the high frame rate have been performed with a series of Airy patterns images compared with an image recorded using the standard BSI-CDD already in operation at the SEXTANTS beamline.
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| 8. |
- O'Shea, James N., et al.
(författare)
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Exploring ultra-fast charge transfer and vibronic coupling with N 1s RIXS maps of an aromatic molecule coupled to a semiconductor
- 2017
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 147:13
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Tidskriftsartikel (refereegranskat)abstract
- We present for the first time two-dimensional resonant inelastic x-ray scattering (RIXS) maps of multilayer and monolayer bi-isonicotinic acid adsorbed on the rutile TiO2(110) single crystal surface. This enables the elastic channel to be followed over the lowest unoccupied molecular orbitals resonantly excited at the N 1s absorption edge. The data also reveal ultra-fast intramolecular vibronic coupling, particularly during excitation into the lowest unoccupied molecular orbital-derived resonance. Both elastic scattering and the vibronic coupling loss features are expected to contain the channel in which the originally excited electron is directly involved in the core-hole decay process. This allows RIXS data for a molecule coupled to a wide bandgap semiconductor to be considered in the same way as the core-hole clock implementation of resonant photoemission spectroscopy (RPES). However, contrary to RPES measurements, we find no evidence for the depletion of the participator channel under the conditions of ultra-fast charge transfer from the molecule to the substrate densities of states, on the time scale of the core-hole lifetime. These results suggest that the radiative core-hole decay processes in RIXS are not significantly modified by charge transfer on the femtosecond time scale in this system.
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| 9. |
- O'Shea, James N., et al.
(författare)
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Ultra-fast intramolecular vibronic coupling revealed by RIXS and RPES maps of an aromatic adsorbate on TiO2(110)
- 2018
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 148:20
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Tidskriftsartikel (refereegranskat)abstract
- Two-dimensional resonant inelastic x-ray scattering (RIXS) and resonant photoelectron spectroscopy (RPES) maps are presented for multilayer and monolayer coverages of an aromatic molecule (bi-isonicotinic acid) on the rutile TiO2(110) single crystal surface. The data reveal ultra-fast intramolecular vibronic coupling upon core excitation from the N 1s orbital into the lowest unoccupied molecular orbital (LUMO) derived resonance. In the RIXS measurements, this results in the splitting of the participator decay channel into a purely elastic line which disperses linearly with excitation energy and a vibronic coupling channel at constant emission energy. In the RPES measurements, the vibronic coupling results in a linear shift in binding energy of the participator channel as the excitation is tuned over the LUMO-derived resonance. Localisation of the vibrations on the molecule on the femtosecond time scale results in predominantly inelastic scattering from the core-excited state in both the physisorbed multilayer and the chemisorbed monolayer.
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| 10. |
- Parra, Erick O. Burgos, et al.
(författare)
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Holographic Magnetic Imaging of Single-Layer Nanocontact Spin-Transfer Oscillators
- 2016
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Ingår i: IEEE transactions on magnetics. - : IEEE. - 0018-9464 .- 1941-0069. ; 52:7
-
Tidskriftsartikel (refereegranskat)abstract
- Time-averaged images of the magnetization within single-layer spin-transfer oscillators have been obtained using the holography with extended reference by autocorrelation linear differential operator technique. Transport measurements on a Pd(5)-Cu(20)-Ni81Fe19(7)-Cu(2)-Pd(2) (in nanometers) stack with a 100 nm diameter nanocontact reveal the presence of vortex dynamics. Magnetic images of the device for injected current values of 24 and -24 mA suggest that a vortex has been ejected from the nanocontact and become pinned at the edge of the region that is visible through the Au mask.
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| 11. |
- Shen, Yazhou, et al.
(författare)
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Characterization of Dynamics in a Premixed Flame
- 2020
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Ingår i: ERCOFTAC Workshop Direct and Large Eddy Simulation. - Cham : Springer. ; , s. 191-197
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Konferensbidrag (refereegranskat)abstract
- The dynamics of a lean premixed flame is investigated using LES. The instantaneous fields show a V-shaped preheat zone while POD results exhibit the dominant single and double helix structures, which contribute to the rotational motion.
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| 12. |
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| 13. |
- Temperton, Robert H., et al.
(författare)
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Resonant inelastic X-ray scattering of a Ru photosensitizer : Insights from individual ligands to the electronic structure of the complete molecule
- 2019
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 151:7
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Tidskriftsartikel (refereegranskat)abstract
- N 1s Resonant Inelastic X-ray Scattering (RIXS) was used to probe the molecular electronic structure of the ruthenium photosensitizer complex cis-bis(isothiocyanato) bis(2,2′-bipyridyl-4,4′-dicarboxylato) ruthenium(II), known as "N3." In order to interpret these data, crystalline powder samples of the bipyridine-dicarboxylic acid ligand ("bi-isonicotinic acid") and the single ring analog "isonicotinic acid" were studied separately using the same method. Clear evidence for intermolecular hydrogen bonding is observed for each of these crystalline powders, along with clear vibronic coupling features. For bi-isonicotinic acid, these results are compared to those of a physisorbed multilayer, where no hydrogen bonding is observed. The RIXS of the "N3" dye, again prepared as a bulk powder sample, is interpreted in terms of the orbital contributions of the bi-isonicotinic acid and thiocyanate ligands by considering the two different nitrogen species. This allows direct comparison with the isolated ligand molecules where we highlight the impact of the central Ru atom on the electronic structure of the ligand. Further interpretation is provided through complementary resonant photoemission spectroscopy and density functional theory calculations. This combination of techniques allows us to confirm the localization and relative coupling of the frontier orbitals and associated vibrational losses.
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| 14. |
- Vodungbo, Boris, et al.
(författare)
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Indirect excitation of ultrafast demagnetization.
- 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
- Does the excitation of ultrafast magnetization require direct interaction between the photons of the optical pump pulse and the magnetic layer? Here, we demonstrate unambiguously that this is not the case. For this we have studied the magnetization dynamics of a ferromagnetic cobalt/palladium multilayer capped by an IR-opaque aluminum layer. Upon excitation with an intense femtosecond-short IR laser pulse, the film exhibits the classical ultrafast demagnetization phenomenon although only a negligible number of IR photons penetrate the aluminum layer. In comparison with an uncapped cobalt/palladium reference film, the initial demagnetization of the capped film occurs with a delayed onset and at a slower rate. Both observations are qualitatively in line with energy transport from the aluminum layer into the underlying magnetic film by the excited, hot electrons of the aluminum film. Our data thus confirm recent theoretical predictions.
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| 15. |
- Zhou Hagström, Nanna, 1993-, et al.
(författare)
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Megahertz-rate Ultrafast X-ray Scattering and Holographic Imaging at the European XFEL
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Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
- The advent of X-ray free-electron lasers (XFELs) has revolutionized fundamental science, from atomic to condensed matter physics, from chemistry to biology, giving researchers access to X-rays with unprecedented brightness, coherence, and pulse duration. All XFEL facilities built until recently provided X-ray pulses at a relatively low repetition rate, with limited data statistics. Here, we present the results from the first megahertz repetition rate X-ray scattering experiments at the Spectroscopy and Coherent Scattering (SCS) instrument of the European XFEL. We illustrate the experimental capabilities that the SCS instrument offers, resulting from the operation at MHz repetition rates and the availability of the novel DSSC 2D imaging detector. Time-resolved magnetic X-ray scattering and holographic imaging experiments in solid state samples were chosen as representative examples, providing an ideal test-bed for operation at megahertz rates. Nevertheless, our results are relevant and applicable to any other non-destructive XFEL experiments in the soft X-ray range.
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| 16. |
- Zhou Hagström, Nanna, 1993-, et al.
(författare)
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Megahertz-rate ultrafast X-ray scattering and holographic imaging at the European XFEL
- 2022
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Ingår i: Journal of Synchrotron Radiation. - : International Union of Crystallography (IUCr). - 0909-0495 .- 1600-5775. ; 29, s. 1454-1464
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Tidskriftsartikel (refereegranskat)abstract
- The advent of X-ray free-electron lasers (XFELs) has revolutionized fundamental science, from atomic to condensed matter physics, from chemistry to biology, giving researchers access to X-rays with unprecedented brightness, coherence and pulse duration. All XFEL facilities built until recently provided X-ray pulses at a relatively low repetition rate, with limited data statistics. Here, results from the first megahertz-repetition-rate X-ray scattering experiments at the Spectroscopy and Coherent Scattering (SCS) instrument of the European XFEL are presented. The experimental capabilities that the SCS instrument offers, resulting from the operation at megahertz repetition rates and the availability of the novel DSSC 2D imaging detector, are illustrated. Time-resolved magnetic X-ray scattering and holographic imaging experiments in solid state samples were chosen as representative, providing an ideal test-bed for operation at megahertz rates. Our results are relevant and applicable to any other non-destructive XFEL experiments in the soft X-ray range.
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