Electron Transfer in a Virtual Quantum State of LiBH4 Induced by Strong Optical Fields and Mapped by Femtosecond X-Ray Diffraction

J. Stingl, F. Zamponi, B. Freyer, M. Woerner, T. Elsaesser, and A. Borgschulte
Phys. Rev. Lett. 109, 147402 – Published 2 October 2012

Abstract

Transient polarizations connected with a spatial redistribution of electronic charge in a mixed quantum state are induced by optical fields of high amplitude. We determine for the first time the related transient electron density maps, applying femtosecond x-ray powder diffraction as a structure probe. The prototype ionic material LiBH4 driven nonresonantly by an intense sub-40 fs optical pulse displays a large-amplitude fully reversible electron transfer from the BH4 anion to the Li+ cation during excitation. Our results establish this mechanism as the source of the strong optical polarization which agrees quantitatively with theoretical estimates.

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  • Received 9 May 2012

DOI:https://doi.org/10.1103/PhysRevLett.109.147402

© 2012 American Physical Society

Authors & Affiliations

J. Stingl1, F. Zamponi1, B. Freyer1, M. Woerner1, T. Elsaesser1, and A. Borgschulte2

  • 1Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie, 12489 Berlin, Germany
  • 2EMPA, Swiss Federal Laboratories for Materials Testing and Research, Laboratory for Hydrogen and Energy, CH-8600 Dübendorf, Switzerland

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Issue

Vol. 109, Iss. 14 — 5 October 2012

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