• Medientyp: E-Artikel
  • Titel: Ultrafast large-amplitude relocation of electronic charge in ionic crystals
  • Beteiligte: Zamponi, Flavio; Rothhardt, Philip; Stingl, Johannes; Woerner, Michael; Elsaesser, Thomas
  • Erschienen: Proceedings of the National Academy of Sciences, 2012
  • Erschienen in: Proceedings of the National Academy of Sciences
  • Sprache: Englisch
  • DOI: 10.1073/pnas.1108206109
  • ISSN: 0027-8424; 1091-6490
  • Schlagwörter: Multidisciplinary
  • Entstehung:
  • Anmerkungen:
  • Beschreibung: <jats:p> The interplay of vibrational motion and electronic charge relocation in an ionic hydrogen-bonded crystal is mapped by X-ray powder diffraction with a 100 fs time resolution. Photoexcitation of the prototype material KH <jats:sub>2</jats:sub> PO <jats:sub>4</jats:sub> induces coherent low-frequency motions of the PO <jats:sub>4</jats:sub> tetrahedra in the electronically excited state of the crystal while the average atomic positions remain unchanged. Time-dependent maps of electron density derived from the diffraction data demonstrate an oscillatory relocation of electronic charge with a spatial amplitude two orders of magnitude larger than the underlying vibrational lattice motions. Coherent longitudinal optical and tranverse optical phonon motions that dephase on a time scale of several picoseconds, drive the charge relocation, similar to a soft (transverse optical) mode driven phase transition between the ferro- and paraelectric phase of KH <jats:sub>2</jats:sub> PO <jats:sub>4</jats:sub> . </jats:p>
  • Zugangsstatus: Freier Zugang