Photoemission of an electron is commonly treated as a one-particle phenomenon. With attosecond streaking spectroscopy we observe the breakdown of this single active-electron approximation by recording up to six attoseconds retardation of the dislodged photoelectron due to electronic correlations. We recorded the photon-energy-dependent emission timing of electrons, released from the helium ground state by an extreme-ultraviolet photon, either leaving the ion in its ground state or exciting it into a shake-up state. We identify an optical field-driven d.c. Stark shift of charge-asymmetric ionic states formed after the entangled photoemission as a key contribution to the observed correlation time shift. These findings enable a complete wavepacket reconstruction and are universal for all polarized initial and final states. Sub-attosecond agreement with quantum mechanical ab initio modelling allows us to determine the absolute zero of time in the photoelectric effect to a precision better than 1/25th of the atomic unit of time.
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We acknowledge insightful comments and generous infrastructural support from F. Krausz. This work was supported by the Max Planck Society, the Deutsche Forschungsgemeinschaft Cluster of Excellence: Munich Centre for Advanced Photonics (http://www.munich-photonics.de), the Austrian Science Foundation project NEXTLITE (F049 and P23359-N16) and LASERLAB-EUROPE (grant agreement no. 654148, European Union’s Horizon 2020 research and innovation programme). J.F. acknowledges funding by the European Research Council (ERC-2011-AdG Proposal 290981). R.K. acknowledges a Consolidator Grant from the European Research Council (ERC-2014-CoG AEDMOS). M.S. was supported by a Marie Curie International Outgoing Fellowship (FP7-PEOPLE-2011-IOF). The computational results presented have been achieved (in part) using the Vienna Scientific Cluster (VSC).
The authors declare no competing financial interests.
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Ossiander, M., Siegrist, F., Shirvanyan, V. et al. Attosecond correlation dynamics. Nature Phys 13, 280–285 (2017). https://doi.org/10.1038/nphys3941
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