Activation of coherent lattice phonon following ultrafast molecular spin-state photo-switching: A molecule-to-lattice energy transfer

  • A. Marino
    Institute de Physique de Rennes 1 , UMR 6251 University Rennes 1-CNRS, 35042 Rennes, France
  • M. Cammarata
    Institute de Physique de Rennes 1 , UMR 6251 University Rennes 1-CNRS, 35042 Rennes, France
  • S. F. Matar
    Université de Bordeaux 2 CNRS, , ICMCB, 87 avenue du Dr. A. Schweitzer, Pessac 33608, France
  • J.-F. Létard
    Université de Bordeaux 2 CNRS, , ICMCB, 87 avenue du Dr. A. Schweitzer, Pessac 33608, France
  • G. Chastanet
    Université de Bordeaux 2 CNRS, , ICMCB, 87 avenue du Dr. A. Schweitzer, Pessac 33608, France
  • M. Chollet
    SLAC National Laboratory 3 LCLS, , Menlo Park, California 94025, USA
  • J. M. Glownia
    SLAC National Laboratory 3 LCLS, , Menlo Park, California 94025, USA
  • H. T. Lemke
    SLAC National Laboratory 3 LCLS, , Menlo Park, California 94025, USA
  • E. Collet
    Institute de Physique de Rennes 1 , UMR 6251 University Rennes 1-CNRS, 35042 Rennes, France

説明

<jats:p>We combine ultrafast optical spectroscopy with femtosecond X-ray absorption to study the photo-switching dynamics of the [Fe(PM-AzA)2(NCS)2] spin-crossover molecular solid. The light-induced excited spin-state trapping process switches the molecules from low spin to high spin (HS) states on the sub-picosecond timescale. The change of the electronic state (&lt;50 fs) induces a structural reorganization of the molecule within 160 fs. This transformation is accompanied by coherent molecular vibrations in the HS potential and especially a rapidly damped Fe-ligand breathing mode. The time-resolved studies evidence a delayed activation of coherent optical phonons of the lattice surrounding the photoexcited molecules.</jats:p>

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