Electron transfer in a virtual quantum state of LiBH4 induced by strong optical fields and mapped by femtosecond x-ray diffraction

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 pro...

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Bibliographic Details
Published in:Physical review letters Vol. 109; no. 14; p. 147402
Main Authors: Stingl, J, Zamponi, F, Freyer, B, Woerner, M, Elsaesser, T, Borgschulte, A
Format: Journal Article
Language:English
Published: United States 05-10-2012
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Summary: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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ISSN:1079-7114
DOI:10.1103/PhysRevLett.109.147402