Abstract
High-harmonic spectroscopy provides a unique insight into the electronic structure of atoms and molecules1,2,3,4,5. Although attosecond science holds the promise of accessing the timescale of electron–electron interactions, until now, their signature has not been seen in high-harmonic spectroscopy. We have recorded high-harmonic spectra of atoms to beyond 160 eV, using a new, almost ideal laser source with a wavelength of 1.8 μm and a pulse duration of less than two optical cycles. We show that we can relate these spectra to differential photoionization cross-sections measured with synchrotron sources. In addition, we show that the high-harmonic spectra contain features due to collective multi-electron effects involving inner-shell electrons, in particular the giant resonance in xenon. We develop a new theoretical model based on the strong-field approximation and show that it is in agreement with the experimental observations.
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Change history
07 March 2011
In the version of this Letter originally published online, the affiliation for the first author, A. D. Shiner, was given incorrectly. This has now been corrected for all versions of the Letter.
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Acknowledgements
The authors thank laser technicians F. Poitras and A. Laramée for their dedicated work on the laser system, and gratefully acknowledge financial support from NSERC, AFOSR, CIPI and FQRNT. We thank U. Becker, M. Spanner and T. Starace for illuminating discussions.
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A.D.S. and B.E.S. contributed equally to this work. B.E.S., F.L. and J-C.K. developed the laser source. A.D.S., B.E.S. and C.T.H. carried out the experiments. H.J.W. interpreted the xenon results. A.D.S. analysed the data. S.P. and D.M.V. provided the theoretical parts. A.D.S., H.J.W., P.B.C. and D.M.V. wrote the manuscript.
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Shiner, A., Schmidt, B., Trallero-Herrero, C. et al. Probing collective multi-electron dynamics in xenon with high-harmonic spectroscopy. Nature Phys 7, 464–467 (2011). https://doi.org/10.1038/nphys1940
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DOI: https://doi.org/10.1038/nphys1940
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