Making the molecular movie with atomic-scale spatial resolution and femtosecond/attosecond-scale time resolution

• Applicant: Dr. Arnaud Rouzée
• Subject Area: Optics, Quantum Optics and Physics of Atoms, Molecules and Plasmas ; Physical Chemistry of Molecules, Liquids and Interfaces, Biophysical Chemistry
• Term: from 2013 to 2018
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 233252030

• Final Report Year: 2019

Final Report Abstract

In summary, we have demonstrated the possibility to generate a broadband, soft X-ray pulse from 70 eV to 150 eV, with an attosecond pulse duration, using a combined 800 nm+1300 nm laser scheme. Using tunable mid-infrared laser pulses, the source was extended to provide ultrashort soft X-ray pulses with a photon energy above the nitrogen K-edge. The source was used to investigate the laser-induced molecular alignment dynamics of CF3I and we were able to distinguish the role of shape resonances in XUV photoionization of aligned molecules. The source was also used to perform static and time-resolved X-ray absorption spectroscopy in gas, liquid and solid targets. We have also provided the first demonstration that time-resolved core-shell photoelectron spectroscopy can be used to investigate ultrafast molecular processes at a free electron laser3. We are therefore convinced that the scheme that has been developed in this proposal to generate ultrashort pulses of short wavelength radiation will be extremely useful in the near future to pursue our investigation of photoinduced molecular dynamics by means of time-resolved photoelectron spectroscopy and diffraction and as well to develop new opportunities to explore ultrafast processes in condensed phase.

Publications

• „Bright attosecond soft X-ray pulse trains by transient phase-matching in two-color highorder harmonic generation“, Optics Express, 23, 248407, (2015)
  Bernd Schütte, Paul Weber, Katalin Kovács, Emeric Balogh, Balázs Major, Valer Tosa, Songhee Han, Marc J. J. Vrakking, katalin Varjú, and Arnaud Rouzée
  
• “Ultrafast modulation of electronic structure by coherent phonon excitations“, Physical Review B, 95, 081101(R), (2017)
  Jannick Weisshaupt, Arnaud Rouzée, Michael Woerner, Marc J. J. Vrakking, Thomas Elsaesser, Eric L. Shirley and Andreas Borgschulte
  
• ”Alignment, orientation and Coulomb explosion of difluoroiodobenzene studied with the pixel imaging mass spectrometry (PimMS) camera", Chem. Phys., 147, 013933, (2017)
  K. Amini et al.
  
• ”Coulomb explosion imaging of concurrent CH2BrI photodissociation dynamics”, Phys. Rev. A, 96, 043415, (2017)
  M. Burt et al
  
• ”Jitter-correction for IR/UV-XUV pump-probe experiments at the FLASH free-electron laser”, New J. Phys., 19, 043009, (2017)
  E. Savelyev et al.
  
• “Photodissociation of aligned CH3I and C6H3F2I molecules probed with time-resolved Coulomb explosion imaging by site-selective extreme ultraviolet ionization”, Struc. Dyn., 5, 014301, (2018)
  K. Amini et al.
  
• “Spectral shift and asymmetries in mid-infrared assisted high-order harmonic generation”, J. Opt. Soc. Am. B, 35, A32-A38, (2018)
  Balázs Major, Emeric Balogh, Katalin Kovács, Songhee Han, Bernd Schütte, Paul Weber, Marc J. J. Vrakking, Valer Tosa, Arnaud Rouzée and katalin Varjú
  
• “Time-resolved inner-shell photoelectron spectroscopy: from a bound molecule to an isolated atom”, Phys. Rev. A, 97, 043429, (2018)
  Felix Brauße et al.
  
• ”Coulomb explosion Imaging of CH3I and CH2ClI photodissociation dynamics”, J. Chem. Phys., 149, 204313, (2018)
  F. Allum et al.
  
• ”Soft X-ray absorption spectroscopy of aqueous solutions using a table-top femtosecond Soft X-ray source”, J. Phys. Chem. Lett., 10, 52, (2019)
  Carlo Kleine, Maria Ekimova, Gildas Goldsztejn, Sebastian Raabe, Christian Strüber, Jan Ludwig, Suresh Yarlagadda, Stefan Eisebitt, Marc J J Vrakking, Thomas Elsaesser, Arnaud Rouzée