| 1. |
- Barillot, T., et al.
(author)
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Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule
- 2021
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In: Physical Review X. - : American Physical Society. - 2160-3308. ; 11:3
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Journal article (peer-reviewed)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. |
- Grånäs, Oscar, 1979-, et al.
(author)
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Ultrafast modification of the electronic structure of a correlated insulator
- 2022
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In: Physical Review Research. - : American Physical Society. - 2643-1564. ; 4:3
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Journal article (peer-reviewed)abstract
- A nontrivial balance between Coulomb repulsion and kinematic effects determines the electronic structure of correlated electron materials. The use of electromagnetic fields strong enough to rival these native microscopic interactions allows us to study the electronic response as well as the time scales and energies involved in using quantum effects for possible applications. We use element-specific transient x-ray absorption spectroscopy and high-harmonic generation to measure the response to ultrashort off-resonant optical fields in the prototypical correlated electron insulator NiO. Surprisingly, fields of up to 0.22 V/angstrom lead to no detectable changes in the correlated Ni 3d orbitals contrary to previous predictions. A transient directional charge transfer is uncovered, a behavior that is captured by first-principles theory. Our results highlight the importance of retardation effects in electronic screening and pinpoints a key challenge in functionalizing correlated materials for ultrafast device operation.
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| 3. |
- John Mukkattukavil, D., et al.
(author)
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Resonant inelastic soft x-ray scattering on LaPt 2 Si 2
- 2022
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In: Journal of physics. Condensed matter : an Institute of Physics journal. - 1361-648X .- 0953-8984. ; 34:32
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Journal article (peer-reviewed)abstract
- X-ray absorption and resonant inelastic x-ray scattering spectra of LaPt2Si2single crystal at the Si 2pand La 4dedges are presented. The data are interpreted in terms of density functional theory, showing that the Si spectra can be described in terms of Sisanddlocal partial density of states (LPDOS), and the La spectra are due to quasi-atomic local 4fexcitations. Calculations show that Ptd-LPDOS dominates the occupied states, and a sharp localized Lafstate is found in the unoccupied states, in line with the observations.
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| 4. |
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| 5. |
- Li, S., et al.
(author)
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Two-dimensional correlation analysis for x-ray photoelectron spectroscopy
- 2021
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In: Journal of Physics B. - : Institute of Physics Publishing (IOPP). - 0953-4075 .- 1361-6455. ; 54:14
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Journal article (peer-reviewed)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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| 6. |
- Eichmann, U., et al.
(author)
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Photon-recoil imaging : Expanding the view of nonlinear x-ray physics
- 2020
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In: Science. - : AMER ASSOC ADVANCEMENT SCIENCE. - 0036-8075 .- 1095-9203. ; 369:6511, s. 1630-1633
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Journal article (peer-reviewed)abstract
- Addressing the ultrafast coherent evolution of electronic wave functions has long been a goal of nonlinear x-ray physics. A first step toward this goal is the investigation of stimulated x-ray Raman scattering (SXRS) using intense pulses from an x-ray free-electron laser. Earlier SXRS experiments relied on signal amplification during pulse propagation through dense resonant media. By contrast, our method reveals the fundamental process in which photons from the primary radiation source directly interact with a single atom. We introduce an experimental protocol in which scattered neutral atoms rather than scattered photons are detected. We present SXRS measurements at the neon K edge and a quantitative theoretical analysis. The method should become a powerful tool in the exploration of nonlinear x-ray physics.
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