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Attosecond correlation dynamics

Nature Physics volume 13, pages 280–285 (2017)Cite this article

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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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References

  1. Einstein, A. Über einen die Erzeugung und Verwandlung des Lichtes betreffenden heuristischen Gesichtspunkt. Ann. Phys. 322, 132–148 (1905).

    Article  Google Scholar 

  2. Schultze, M. et al. Delay in photoemission. Science 328, 1658–1662 (2010).

    Article  ADS  Google Scholar 

  3. Klünder, K. et al. Probing single-photon ionization on the attosecond time scale. Phys. Rev. Lett. 106, 143002 (2011).

    Article  ADS  Google Scholar 

  4. Eckle, P. et al. Attosecond ionization and tunneling delay time measurements in helium. Science 322, 1525–1529 (2008).

    Article  ADS  Google Scholar 

  5. Sabbar, M. et al. Resonance effects in photoemission time delays. Phys. Rev. Lett. 115, 133001 (2015).

    Article  ADS  Google Scholar 

  6. Palatchi, C. et al. Atomic delay in helium, neon, argon and krypton. J. Phys. B 47, 245003 (2014).

    Article  ADS  Google Scholar 

  7. Wigner, E. P. Lower limit for the energy derivative of the scattering phase shift. Phys. Rev. 98, 145–147 (1955).

    Article  ADS  MathSciNet  Google Scholar 

  8. Eisenbud, L. The Formal Properties of Nuclear Collisions (Princeton Univ., 1948).

    Google Scholar 

  9. Smith, F. T. Lifetime matrix in collision theory. Phys. Rev. 118, 349–356 (1960).

    Article  ADS  MathSciNet  Google Scholar 

  10. Nussenzveig, H. M. Time delay in quantum scattering. Phys. Rev. D 6, 1534–1542 (1972).

    Article  ADS  Google Scholar 

  11. de Carvalho, C. A. A. & Nussenzveig, H. M. Time delay. Phys. Rep. 364, 83–174 (2002).

    Article  ADS  MathSciNet  Google Scholar 

  12. Sassoli de Bianchi, M. Time-delay of classical and quantum scattering processes: a conceptual overview and a general definition. Centr. Eur. J. Phys. 10, 282–319 (2012).

    ADS  Google Scholar 

  13. Tew, D. P., Klopper, W. & Helgaker, T. Electron correlation: the many-body problem at the heart of chemistry. J. Comput. Chem. 28, 1307–1320 (2007).

    Article  Google Scholar 

  14. Fulde, P. Electron Correlations in Molecules and Solids (Springer Science & Business Media, 2012).

    MATH  Google Scholar 

  15. Datta, S. Electronic Transport in Mesoscopic Systems (Cambridge Univ. Press, 1997).

    Google Scholar 

  16. Auerbach, A. Interacting Electrons and Quantum Magnetism (Springer, 1994).

    Book  Google Scholar 

  17. Hubbard, J. Electron correlations in narrow energy bands. Proc. R. Soc. Lond. A 276, 238–257 (1963).

    Article  ADS  Google Scholar 

  18. Pazourek, R., Feist, J., Nagele, S. & Burgdörfer, J. Attosecond streaking of correlated two-electron transitions in helium. Phys. Rev. Lett. 108, 163001 (2012).

    Article  ADS  Google Scholar 

  19. Dahlström, J. M., L’Huillier, A. & Maquet, A. Introduction to attosecond delays in photoionization. J. Phys. B 45, 183001 (2012).

    Article  Google Scholar 

  20. Nagele, S., Pazourek, R., Feist, J. & Burgdörfer, J. Time shifts in photoemission from a fully correlated two-electron model system. Phys. Rev. A 85, 033401 (2012).

    Article  ADS  Google Scholar 

  21. Kheifets, A. S. Time delay in valence-shell photoionization of noble-gas atoms. Phys. Rev. A 87, 063404 (2013).

    Article  ADS  Google Scholar 

  22. Zhang, C.-H. & Thumm, U. Streaking and Wigner time delays in photoemission from atoms and surfaces. Phys. Rev. A 84, 033401 (2011).

    Article  ADS  Google Scholar 

  23. Sukiasyan, S., Ishikawa, K. L. & Ivanov, M. Attosecond cascades and time delays in one-electron photoionization. Phys. Rev. A 86, 033423 (2012).

    Article  ADS  Google Scholar 

  24. Moore, L. R., Lysaght, M. A., Parker, J. S., van der Hart, H. W. & Taylor, K. T. Time delay between photoemission from the 2p and 2s subshells of neon. Phys. Rev. A 84, 061404 (2011).

    Article  ADS  Google Scholar 

  25. Baggesen, J. C. & Madsen, L. Atomic and molecular phases through attosecond streaking. Phys. Rev. A 83, 021403(R) (2011).

    Article  ADS  Google Scholar 

  26. Kheifets, A. S., Saha, S., Deshmukh, P. C., Keating, D. A. & Manson, S. T. Dipole phase and photoelectron group delay in inner-shell photoionization. Phys. Rev. A 92, 063422 (2015).

    Article  ADS  Google Scholar 

  27. Zhang, C.-H. & Thumm, U. Electron-ion interaction effects in attosecond time-resolved photoelectron spectra. Phys. Rev. A 82, 043405 (2010).

    Article  ADS  Google Scholar 

  28. Baggesen, J. C. & Madsen, L. B. Polarization effects in attosecond photoelectron spectroscopy. Phys. Rev. Lett. 104, 043602 (2010).

    Article  ADS  Google Scholar 

  29. Nagele, S. et al. Time-resolved photoemission by attosecond streaking: extraction of time information. J. Phys. B 44, 081001 (2011).

    Article  ADS  Google Scholar 

  30. Heimann, P. A. et al. Helium and neon photoelectron satellites at threshold. Phys. Rev. A 34, 3782–3791 (1986).

    Article  ADS  Google Scholar 

  31. Itatani, J. et al. Attosecond streak camera. Phys. Rev. Lett. 88, 173903 (2002).

    Article  ADS  Google Scholar 

  32. Yakovlev, V. S., Gagnon, J., Karpowicz, N. & Krausz, F. Attosecond streaking enables the measurement of quantum phase. Phys. Rev. Lett. 105, 073001 (2010).

    Article  ADS  Google Scholar 

  33. Feist, J. et al. Nonsequential two-photon double ionization of helium. Phys. Rev. A 77, 043420 (2008).

    Article  ADS  Google Scholar 

  34. Schneider, B. I. et al. Quantum Dynamic Imaging 149–208 (Springer Science & Business Media, 2011).

    Book  Google Scholar 

  35. Ivanov, M. & Smirnova, O. How accurate is the attosecond streak camera? Phys. Rev. Lett. 107, 213605 (2011).

    Article  ADS  Google Scholar 

  36. Palacios, A., McCurdy, C. W. & Rescigno, T. N. Extracting amplitudes for single and double ionization from a time-dependent wave packet. Phys. Rev. A 76, 043420 (2007).

    Article  ADS  Google Scholar 

  37. Woodruff, P. R. & Samson, J. A. R. Measurements of partial cross sections and autoionization in the photoionization of helium to He+ (N = 2). Phys. Rev. A 25, 848–856 (1982).

    Article  ADS  Google Scholar 

  38. Trebino, R. et al. Measuring ultrashort laser pulses in the time-frequency domain using frequency-resolved optical gating. Rev. Sci. 68, 3277–3295 (1997).

    Article  ADS  Google Scholar 

  39. Vampa, G. & Villeneuve, D. M. High-harmonic generation: to the extreme. Nat. Phys. 11, 529–530 (2015).

    Article  Google Scholar 

  40. Luu, T. T. et al. Extreme ultraviolet high-harmonic spectroscopy of solids. Nature 521, 498–502 (2015).

    Article  ADS  Google Scholar 

  41. Ghimire, S. et al. Strong-field and attosecond physics in solids. J. Phys. B 47, 204030 (2014).

    Article  ADS  Google Scholar 

  42. Schultze, M. et al. Attosecond band-gap dynamics in silicon. Science 346, 1348–1352 (2014).

    Article  ADS  Google Scholar 

  43. Ramachandran, P. & Varoquaux, G. Mayavi: 3D visualization of scientific data. Comput. Sci. Eng. 13, 40–51 (2011).

    Article  Google Scholar 

  44. Schweinberger, W. et al. Waveform-controlled near-single-cycle milli-joule laser pulses generate sub-10 nm extreme ultraviolet continua. Opt. Lett. 37, 3573–3575 (2012).

    Article  ADS  Google Scholar 

  45. Corkum, P. B. Plasma perspective on strong-field multiphoton ionization. Phys. Rev. Lett. 71, 1994–1997 (1993).

    Article  ADS  Google Scholar 

  46. Schafer, K. & Kulander, K. High harmonic generation from ultrafast pump lasers. Phys. Rev. Lett. 78, 638–641 (1997).

    Article  ADS  Google Scholar 

  47. Hofstetter, M. et al. Lanthanum–molybdenum multilayer mirrors for attosecond pulses between 80 and 130 eV. New J. Phys. 13, 063038 (2011).

    Article  ADS  Google Scholar 

  48. Mairesse, Y. et al. Attosecond synchronization of high-harmonic soft x-rays. Science 302, 1540–1543 (2003).

    Article  ADS  Google Scholar 

  49. Fiess, M. et al. Versatile apparatus for attosecond metrology and spectroscopy. Rev. Sci. 81, 093103 (2010).

    Article  ADS  Google Scholar 

  50. Becker, U. & Shirley, D. A. VUV and Soft X-ray Photoionization (Springer Science & Business Media, 2012).

    Google Scholar 

Download references

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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Authors and Affiliations

  1. Max-Planck-Institut für Quantenoptik, Hans-Kopfermann-Strasse 1, 85748 Garching, Germany

    M. Ossiander, F. Siegrist, V. Shirvanyan, A. Sommer, T. Latka, A. Guggenmos, R. Kienberger & M. Schultze

  2. Physik-Department, Technische Universität München, James-Franck-Strasse 1, 85748 Garching, Germany

    M. Ossiander, F. Siegrist, V. Shirvanyan, T. Latka & R. Kienberger

  3. Institute for Theoretical Physics, Vienna University of Technology, Wiedner Hauptstrasse 8-10, 1040 Vienna, Austria

    R. Pazourek, S. Nagele & J. Burgdörfer

  4. Fakultät für Physik, Ludwig-Maximilians-Universität München, Am Coulombwall 1, 85748 Garching, Germany

    A. Guggenmos & M. Schultze

  5. Departamento de Física Teórica de la Materia Condensada and Condensed Matter Physics Center (IFIMAC), Universidad Autónoma de Madrid, 28049 Madrid, Spain

    J. Feist

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  1. M. Ossiander
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Contributions

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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