Abstract
All properties of molecules—from binding and excitation energies to their geometry—are determined by the highly correlated initial-state wavefunction of the electrons and nuclei. Details of these correlations can be revealed by studying the break-up of these systems into their constituents. The fragmentation might be initiated by the absorption of a single photon1,2,3,4,5,6, by collision with a charged particle7,8 or by exposure to a strong laser pulse9,10: if the interaction causing the excitation is sufficiently understood, the fragmentation process can then be used as a tool to investigate the bound initial state11,12. The interaction and resulting fragment motions therefore pose formidable challenges to quantum theory13,14,15. Here we report the coincident measurement of the momenta of both nuclei and both electrons from the single-photon-induced fragmentation of the deuterium molecule. The results reveal that the correlated motion of the electrons is strongly dependent on the inter-nuclear separation in the molecular ground state at the instant of photon absorption.
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Acknowledgements
We thank Roentdek GmbH (http://www.Roentdek.com) for support with detectors, and acknowledge helpful discussion with colleagues M. Walter, J. Briggs, J. Feagin, T. Reddish and V. Schmidt. This work was supported by the Deutsche Forschungs Gemeinschaft, the Bundesministerium für Bildung und Forschung, and the Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, US Department of Energy (DOE). T.W. thanks Graduiertenförderung des Landes Hessen, the Alexander von Humboldt Stiftung and the Herrmann Willkomm Stiftung for financial support.
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Weber, T., Czasch, A., Jagutzki, O. et al. Complete photo-fragmentation of the deuterium molecule. Nature 431, 437–440 (2004). https://doi.org/10.1038/nature02839
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DOI: https://doi.org/10.1038/nature02839
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