| 1. |
- Canton, Sophie, et al.
(författare)
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Visualizing the non-equilibrium dynamics of photoinduced intramolecular electron transfer with femtosecond X-ray pulses.
- 2015
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 6
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Tidskriftsartikel (refereegranskat)abstract
- Ultrafast photoinduced electron transfer preceding energy equilibration still poses many experimental and conceptual challenges to the optimization of photoconversion since an atomic-scale description has so far been beyond reach. Here we combine femtosecond transient optical absorption spectroscopy with ultrafast X-ray emission spectroscopy and diffuse X-ray scattering at the SACLA facility to track the non-equilibrated electronic and structural dynamics within a bimetallic donor-acceptor complex that contains an optically dark centre. Exploiting the 100-fold increase in temporal resolution as compared with storage ring facilities, these measurements constitute the first X-ray-based visualization of a non-equilibrated intramolecular electron transfer process over large interatomic distances. Experimental and theoretical results establish that mediation through electronically excited molecular states is a key mechanistic feature. The present study demonstrates the extensive potential of femtosecond X-ray techniques as diagnostics of non-adiabatic electron transfer processes in synthetic and biological systems, and some directions for future studies, are outlined.
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| 2. |
- Fukuzawa, Hironobu, et al.
(författare)
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Real-time observation of X-ray-induced intramolecular and interatomic electronic decay in CH2I2
- 2019
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 10:1
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Tidskriftsartikel (refereegranskat)abstract
- The increasing availability of X-ray free-electron lasers (XFELs) has catalyzed the development of single-object structural determination and of structural dynamics tracking in real-time. Disentangling the molecular-level reactions triggered by the interaction with an XFEL pulse is a fundamental step towards developing such applications. Here we report real-time observations of XFEL-induced electronic decay via short-lived transient electronic states in the diiodomethane molecule, using a femtosecond near-infrared probe laser. We determine the lifetimes of the transient states populated during the XFEL-induced Auger cascades and find that multiply charged iodine ions are issued from short-lived (∼20 fs) transient states, whereas the singly charged ones originate from significantly longer-lived states (∼100 fs). We identify the mechanisms behind these different time scales: contrary to the short-lived transient states which relax by molecular Auger decay, the long-lived ones decay by an interatomic Coulombic decay between two iodine atoms, during the molecular fragmentation. © 2019, The Author(s).
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| 3. |
- Giorgianni, Flavio, et al.
(författare)
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Melting of magnetic order in NaOsO3 by femtosecond laser pulses
- 2022
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Ingår i: Physical Review B. - : American Physical Society. - 2469-9950 .- 2469-9969. ; 105:15
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Tidskriftsartikel (refereegranskat)abstract
- NaOsO3 has recently attracted significant attention for the strong coupling between its electronic band structure and magnetic ordering. Here, we used time-resolved magnetic x-ray diffraction to determine the timescale of the photoinduced antiferromagnetic dynamics in NaOsO3. Our measurements are consistent with a sub-100 fs melting of the antiferromagnetic long-range order that occurs significantly faster than the lattice dynamics as monitored by the transient change in intensity of selected Bragg structural reflections, which instead show a decrease of intensity on a timescale of several ps.
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| 4. |
- Kim, Kyung Hwan, et al.
(författare)
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Anisotropic X-Ray Scattering of Transiently Oriented Water
- 2020
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Ingår i: Physical Review Letters. - : American Physical Society (APS). - 0031-9007 .- 1079-7114. ; 125:7
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Tidskriftsartikel (refereegranskat)abstract
- We study the structural dynamics of liquid water by time-resolved anisotropic x-ray scattering under the optical Kerr effect condition. In this way, we can separate the anisotropic scattering decay of 160 fs from the delayed temperature increase of similar to 0.1 K occurring at 1 ps and quantify transient changes in the O-O pair distribution function. Polarizable molecular dynamics simulations reproduce well the experiment, indicating transient alignment of molecules along the electric field, which shortens the nearest-neighbor distances. In addition, analysis of the simulated water local structure provides evidence that two hypothesized fluctuating water configurations exhibit different polarizability.
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| 5. |
- Kumagai, Yoshiaki, et al.
(författare)
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Suppression of thermal nanoplasma emission in clusters strongly ionized by hard x-rays
- 2021
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Ingår i: Journal of Physics B. - : Institute of Physics Publishing (IOPP). - 0953-4075 .- 1361-6455. ; 54:4
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Tidskriftsartikel (refereegranskat)abstract
- Using electron and ion spectroscopy, we studied the electron and nuclear dynamics in similar to 50 000-atom large krypton clusters, following excitation with an intense hard x-ray pulse. Beyond the single pulse experiment, we also present the results of a time-resolved, x-ray pump-near-infrared probe measurement that allows one to learn about the time evolution of the system. After core ionization of the atoms by x-ray photons, trapped Auger and secondary electrons form a nanoplasma in which the krypton ions are embedded, according to the already published scenario. While the ion data show expected features, the electron emission spectra miss the expected pump-probe delay-dependent enhancement except for a slight enhancement in the energy range below 2 eV. Theoretical simulations help to reveal that, due to the deep trapping potential of the ions during the long time expansion accompanied by electron-ion recombination, thermal emission from the transient nanoplasma becomes quenched.
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| 6. |
- Milne, Christopher J., et al.
(författare)
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Disentangling the evolution of electrons and holes in photoexcited ZnO nanoparticles
- 2023
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Ingår i: Structural Dynamics. - : American Institute of Physics (AIP). - 2329-7778. ; 10:6
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Tidskriftsartikel (refereegranskat)abstract
- The evolution of charge carriers in photoexcited room temperature ZnO nanoparticles in solution is investigated using ultrafast ultraviolet photoluminescence spectroscopy, ultrafast Zn K-edge absorption spectroscopy, and ab initio molecular dynamics (MD) simulations. The photoluminescence is excited at 4.66 eV, well above the band edge, and shows that electron cooling in the conduction band and exciton formation occur in <500 fs, in excellent agreement with theoretical predictions. The x-ray absorption measurements, obtained upon excitation close to the band edge at 3.49 eV, are sensitive to the migration and trapping of holes. They reveal that the 2 ps transient largely reproduces the previously reported transient obtained at 100 ps time delay in synchrotron studies. In addition, the x-ray absorption signal is found to rise in similar to 1.4 ps, which we attribute to the diffusion of holes through the lattice prior to their trapping at singly charged oxygen vacancies. Indeed, the MD simulations show that impulsive trapping of holes induces an ultrafast expansion of the cage of Zn atoms in <200 fs, followed by an oscillatory response at a frequency of similar to 100 cm-1, which corresponds to a phonon mode of the system involving the Zn sub-lattice.
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| 7. |
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| 8. |
- Yamamoto, Kohei, et al.
(författare)
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Ultrafast demagnetization of Pt magnetic moment in L1(0)-FePt probed by magnetic circular dichroism at a hard x-ray free electron laser
- 2019
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Ingår i: New Journal of Physics. - : IOP PUBLISHING LTD. - 1367-2630. ; 21:12
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Tidskriftsartikel (refereegranskat)abstract
- Unraveling the origin of ultrafast demagnetization in multisublattice ferromagnetic materials requires femtosecond x-ray techniques to trace the magnetic moment dynamics on individual elements, but this could not yet be achieved in the hard x-ray regime. We demonstrate here the first ultrafast demagnetization dynamics in the ferromagnetic heavy 5d-transition metal Pt using circularly-polarized hard x-rays at an x-ray free electron laser (XFEL). The decay time of laser-induced demagnetization of L1(0)-FePt is determined to be tau(Pt) = 0.61 +/- 0.04 ps using time-resolved x-ray magnetic circular dichroism at the Pt L-3 edge, whereas magneto-optical Kerr measurements indicate the decay time for the total magnetization as tau(total) < 0.1 ps. A transient magnetic state with a photomodulated ratio of the 3d and 5d magnetic moments is demonstrated for pump-probe delays larger than 1 ps. We explain this distinct photo-modulated transient magnetic state by the induced-moment behavior of the Pt atom and the x-ray probing depth. Our findings pave the way for the future use of XFELs to disentangle atomic spin dynamics contributions.
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