| 1. |
- 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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| 2. |
- 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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| 3. |
- 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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| 4. |
- Grönlund, Rasmus, et al.
(författare)
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Laser-Induced Fluorescence for Assessment of Cultural Heritage
- 2006
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Konferensbidrag (refereegranskat)abstract
- Remote imaging measurements of laser-induced fluorescence have been performed, with application towards cultural heritage. Measurement campaigns have been performed at, e.g., the Coliseum in Rome. Differences in fluorescence spectra from different points were found and images corresponding to different features could be produced for thematic mapping.
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| 5. |
- Grönlund, Rasmus, et al.
(författare)
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Laser-induced fluorescence imaging for studies of cultural heritage - art. no. 66180P
- 2007
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Ingår i: O3A: Optics for Arts, Architecture, and Archaeology. - : SPIE. - 1996-756X .- 0277-786X. - 9780819467607 ; 6618, s. 6180-6180
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Konferensbidrag (refereegranskat)abstract
- Laser-induced fluorescence for remote imaging of historical monuments is an established technique, which in this work has been used in measurement campaigns at the Coliseum and the Baptistery of San Giovanni in Laterano in Rome, Italy. The results presented here are examples that show that biodeteriogens can be monitored and that. materials can be identified. Also, cleaned and soiled areas on the stone can be localized and differences between soiling can be found, which may be useful in the sustainable conservation for mapping and evaluation.
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| 6. |
- Hennecke, Martin, et al.
(författare)
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Ultrafast opto-magnetic effects in the extreme ultraviolet spectral range
- 2024
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Ingår i: Communications Physics. - : Springer Nature. - 2399-3650. ; 7:1
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Tidskriftsartikel (refereegranskat)abstract
- Coherent light-matter interactions mediated by opto-magnetic phenomena like the inverse Faraday effect (IFE) are expected to provide a non-thermal pathway for ultrafast manipulation of magnetism on timescales as short as the excitation pulse itself. As the IFE scales with the spin-orbit coupling strength of the involved electronic states, photo-exciting the strongly spin-orbit coupled core-level electrons in magnetic materials appears as an appealing method to transiently generate large opto-magnetic moments. Here, we investigate this scenario in a ferrimagnetic GdFeCo alloy by using intense and circularly polarized pulses of extreme ultraviolet radiation. Our results reveal ultrafast and strong helicity-dependent magnetic effects which are in line with the characteristic fingerprints of an IFE, corroborated by ab initio opto-magnetic IFE theory and atomistic spin dynamics simulations.
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| 7. |
- Hällström, Jenny, et al.
(författare)
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Documentation of soiled and biodeteriorated facades: a case study on the Coliseum, Rome, using hyperspectral imaging fluorescence lidars
- 2009
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Ingår i: Journal of Cultural Heritage. - : Elsevier BV. - 1778-3674 .- 1296-2074. ; 10:1, s. 106-115
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Tidskriftsartikel (refereegranskat)abstract
- Non-invasive documentation of historic façades with fluorescence lidar techniques can provide helpful information for the cultural heritage sector, especially when large areas outdoors are to be examined. This paper presents a case study on the Coliseum, Rome, where both cleaned and heavily soiled areas of the monument were scanned and analysed with two fluorescence lidar systems. Biodeterioration processes have also been addressed during the experiment with the aim of assessing the colonisation extent on selected areas of the monument. Results show the usefulness of a mobile fluorescence lidar system for documentation and survey of large surfaces with complex conditions without limiting the public access to the monument.
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| 8. |
- Hällström, Jenny, et al.
(författare)
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Remote fluorescence lidar imaging of monuments: the Coliseum and the Lateran Baptistery in Rome
- 2008
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Ingår i: LASERS IN THE CONSERVATION OF ARTWORKS. - 9780415475969 ; , s. 169-175
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Konferensbidrag (refereegranskat)abstract
- On site remote laser-induced fluorescence measurements have been performed with application towards non-movable objects. This paper describes the application of non-invasive hyperspectral fluorescence imaging to two masonry monuments, the Coliseum and the Lateran Baptistery in Rome, during a joint Italian-Swedish experiment. The mobile systems of Lund Institute of Technology, Sweden, and CNR-IFAC, Italy, were placed at the distance of 18-65 m from the façades for the documentation and characterization of surfaces, including materials, protective treatments, biodeteriogens and historic layers.
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| 9. |
- 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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| 10. |
- Palombi, Lorenzo, et al.
(författare)
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Hyperspectral fluorescence lidar imaging at the Colosseum, Rome
- 2008
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Ingår i: Optics Express. - 1094-4087. ; 16:10, s. 6794-6808
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Tidskriftsartikel (refereegranskat)abstract
- Fluorescence lidar techniques offer considerable potential for remote, non-invasive diagnostics of stone cultural heritage in the outdoor environment. Here we present the results of a joint Italian-Swedish experiment, deploying two hyperspectral fluorescence lidar imaging systems, for the documentation of past conservation interventions on the Colosseum, Rome. Several portions of the monument were scanned and we show that it was possible to discriminate among masonry materials, reinforcement structures and protective coatings inserted during past conservation interventions, on the basis of their fluorescence signatures, providing useful information for a first quick, large-scale in situ screening of the monument.
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| 11. |
- Schreck, Simon, et al.
(författare)
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Atom-Specific Probing of Electron Dynamics in an Atomic Adsorbate by Time-Resolved X-Ray Spectroscopy
- 2022
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Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 129:27
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Tidskriftsartikel (refereegranskat)abstract
- The electronic excitation occurring on adsorbates at ultrafast timescales from optical lasers that initiate surface chemical reactions is still an open question. Here, we report the ultrafast temporal evolution of x-ray absorption spectroscopy (XAS) and x-ray emission spectroscopy (XES) of a simple well-known adsorbate prototype system, namely carbon (C) atoms adsorbed on a nickel [Ni(100)] surface, following intense laser optical pumping at 400 nm. We observe ultrafast (∼100 fs) changes in both XAS and XES showing clear signatures of the formation of a hot electron-hole pair distribution on the adsorbate. This is followed by slower changes on a few picoseconds timescale, shown to be consistent with thermalization of the complete C/Ni system. Density functional theory spectrum simulations support this interpretation.
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| 12. |
- 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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