Attosecond correlation dynamics

Abstract

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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Figure 1: Attosecond streaking spectroscopy of shake-up states in helium.
Figure 2: Absolute timing of the photoelectric (PE) effect in helium.
Figure 3: The d.c. Stark effect at optical frequencies.
Figure 4: Effective dipole moment for the n = 2 shake-up state and relative group delay dispersion of the correlation time.

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Acknowledgements

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).

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Experimental studies and analysis of experimental and theoretical signatures were carried out by M.O., F.S., V.S., A.S., T.L. and M.S. Theory and modelling were performed by R.P., supported by S.N. and J.F., and supervised by J.B. Customized XUV optics were provided by A.G. The manuscript was written by M.O., F.S. and M.S. All authors discussed the results and commented on the paper.

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Correspondence to M. Ossiander or M. Schultze.

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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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