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Probing and controlling non-Born–Oppenheimer dynamics in highly excited molecular ions

Nature Physics volume 8, pages 232237 (2012) | Download Citation

Abstract

In the extreme ultraviolet and soft-X-ray regions of the spectrum, light–matter interaction is dominated by photoionization. In molecular systems, the sudden removal of an electron will initiate ultrafast electronic and nuclear dynamics in the residual molecular ion. A particularly interesting aspect of these dynamics is the correlated motions of electrons and nuclei, an understanding of which lies at the heart of chemistry. Here we use a few-femtosecond high-harmonic pulse and a weak infrared laser pulse to initiate and probe the explosion of a triatomic N2O+ molecular ion in real time, in a regime dominated by coupled electron–electron and electron–nuclear dynamics. We also show that the branching ratio of bond breaking can be altered in the presence of the laser field.

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Acknowledgements

The authors gratefully acknowledge financial support from Department of Energy (DOE) Basic Energy Sciences (BES) Chemical Sciences and used facilities provided by the National Science Foundation Engineering Research Center for Extreme Ultraviolet Science (NSF EUV ERC). We thank O. Vendrell and R. Santra for critical comments of the manuscript, and X-M. Tong illuminating discussions. We also thank A. Czasch and T. Jahnke from RoentDek for the COLTRIMS support, and Y. Liu for providing us the EUV multilayer mirrors.

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Author notes

    • X. Zhou

    Present address: Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA

Affiliations

  1. Department of Physics and JILA, University of Colorado, Boulder, Colorado 80309, USA

    • X. Zhou
    • , P. Ranitovic
    • , C. W. Hogle
    • , H. C. Kapteyn
    •  & M. M. Murnane
  2. Department of Chemistry, Oxford University, South Parks Road, Oxford, OX1 3QZ, UK

    • J. H. D. Eland

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Contributions

X.Z., M.M.M. and H.C.K. conceived the project. X.Z., P.R. and C.W.H. performed the experiments and analysed the data. All authors contributed to the data interpretation and paper.

Competing interests

The authors declare no competing financial interests.

Corresponding authors

Correspondence to X. Zhou or M. M. Murnane.

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https://doi.org/10.1038/nphys2211

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