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Sökning: WFRF:(Coffee R. N.) > (2020-2023)

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1.
  • Perosa, G., et al. (författare)
  • Femtosecond Polarization Shaping of Free-Electron Laser Pulses
  • 2023
  • Ingår i: Physical Review Letters. - 0031-9007. ; 131:4
  • Tidskriftsartikel (refereegranskat)abstract
    • We demonstrate the generation of extreme-ultraviolet (XUV) free-electron laser (FEL) pulses with timedependent polarization. To achieve polarization modulation on a femtosecond timescale, we combine two mutually delayed counterrotating circularly polarized subpulses from two cross-polarized undulators. The polarization profile of the pulses is probed by angle-resolved photoemission and above-threshold ionization of helium; the results agree with solutions of the time-dependent Schrodinger equation. The stability limit of the scheme is mainly set by electron-beam energy fluctuations, however, at a level that will not compromise experiments in the XUV. Our results demonstrate the potential to improve the resolution and element selectivity of methods based on polarization shaping and may lead to the development of new coherent control schemes for probing and manipulating core electrons in matter.
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3.
  • Barillot, T., et al. (författare)
  • Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule
  • 2021
  • Ingår i: Physical Review X. - : American Physical Society. - 2160-3308. ; 11:3
  • Tidskriftsartikel (refereegranskat)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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