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Tunable isolated attosecond X-ray pulses with gigawatt peak power from a free-electron laser

Nature Photonics volume 14, pages 30–36 (2020)Cite this article

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Abstract

The quantum-mechanical motion of electrons in molecules and solids occurs on the sub-femtosecond timescale. Consequently, the study of ultrafast electronic phenomena requires the generation of laser pulses shorter than 1 fs and of sufficient intensity to interact with their target with high probability. Probing these dynamics with atomic-site specificity requires the extension of sub-femtosecond pulses to the soft X-ray spectral region. Here, we report the generation of isolated soft X-ray attosecond pulses with an X-ray free-electron laser. Our source has a pulse energy that is millions of times larger than any other source of isolated attosecond pulses in the soft X-ray spectral region, with a peak power exceeding 100 GW. This unique combination of high intensity, high photon energy and short pulse duration enables the investigation of electron dynamics with X-ray nonlinear spectroscopy and single-particle imaging, unlocking a path towards a new era of attosecond science.

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Fig. 1: Diagram of the XLEAP operation.
Fig. 2: Results of the angular streaking measurement.
Fig. 3: Spectral measurements.
Fig. 4: Comparison to state-of-the-art attosecond sources.
Fig. 5: Double-pulse measurements.

Data availability

A subset of the raw data used to produce Figs. 2–5 is publicly available at figshare (https://figshare.com/projects/Tunable_Isolated_Attosecond_X-ray_Pulses_with_Gigawatt_Peak_Power_from_a_Free-Electron_Laser/65741). This repository also contains a copy of the analysis script used to invert the photoelectron momentum distributions. All other data that support the plots within this paper and other findings of this study are available from the corresponding authors on reasonable request.

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Acknowledgements

We would like to acknowledge T. Gorkhover, C. Bostedt, C. Pellegrini, A. Cavalieri, N. Berrah, L. Young, L. F. DiMauro, H.-D. Nuhn, G. Marcus, T. Maxwell, M. Dunne, M. Minitti and R. Schoenlein for useful discussions and suggestions. We would also like to acknowledge M. Merritt, O. Schmidt, N. Strelnikov and I. Vasserman for their assistance in designing, constructing and installing the XLEAP wiggler. We also acknowledge the SLAC Accelerator Operations and the LCLS operations group, and the Mechanical and Electrical engineering divisions of the SLAC Accelerator Directorate, especially G. Kraft, M. Carrasco, A. Cedillos, K. Luchini, D. Bohler and J. Mock for their invaluable support. This work was supported by US Department of Energy contract nos. DE-AC02-76SF00515, DOE-BES Accelerator and detector research program Field Work Proposal 100317, DOE-BES, Chemical Sciences, Geosciences, and Biosciences Division, and Department of Energy, Laboratory Directed Research and Development program at SLAC National Accelerator Laboratory, under contract DE-AC02-76SF00515. W.H. acknowledges financial support by the BACATEC programme. P.R. and M.F.K. acknowledge additional support by the DFG via KL-1439/10, and the Max Planck Society. G.H. acknowledges the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) Projektnummer 328961117 SFB 1319 ELCH. A.Z. and J.Z.X. acknowledge support by the US Department of Energy contract no. DE-AC02-06CH11357. J.P.Marangos and T.D. acknowledge support by EPSRC programme grant EP/R019509/1.

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Author notes

  1. These authors contributed equally: Joseph Duris, Siqi Li.

Authors and Affiliations

  1. SLAC National Accelerator Laboratory, Menlo Park, CA, USA

    Joseph Duris, Siqi Li, Taran Driver, James P. MacArthur, Alberto A. Lutman, Zhen Zhang, Philipp Rosenberger, Jeff W. Aldrich, Ryan Coffee, Giacomo Coslovich, Franz-Josef Decker, James M. Glownia, Jacek Krzywinski, Ming-Fu Lin, Megan Nantel, Niranjan Shivaram, Peter Walter, James J. Welch, Matthias F. Kling, Philip H. Bucksbaum, Zhirong Huang, James P. Cryan & Agostino Marinelli

  2. Physics Department, Stanford University, Stanford, CA, USA

    Siqi Li, James P. MacArthur, Andrei Kamalov, Megan Nantel, Jordan T. O’Neal & Philip H. Bucksbaum

  3. Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA

    Taran Driver, Elio G. Champenois, Philipp Rosenberger, Andrei Kamalov, Jonas Knurr, Adi Natan, Jordan T. O’Neal, Anna Li Wang, Thomas J. A. Wolf, Matthias F. Kling, Philip H. Bucksbaum & James P. Cryan

  4. The Blackett Laboratory, Imperial College London, London, UK

    Taran Driver & Jon P. Marangos

  5. Max Planck Institute of Quantum Optics, Garching, Germany

    Philipp Rosenberger & Matthias F. Kling

  6. Physics Department, Ludwig-Maximilians-Universität Munich, Garching, Germany

    Philipp Rosenberger, Wolfram Helml & Matthias F. Kling

  7. Institut für Physik und CINSaT, Universität Kassel, Kassel, Germany

    Gregor Hartmann

  8. Zentrum für Synchrotronstrahlung, Technische Universität Dortmund, Dortmund, Germany

    Wolfram Helml

  9. Physik-Department E11, Technische Universität München, Garching, Germany

    Wolfram Helml

  10. Applied Physics Department, Stanford University, Stanford, CA, USA

    Anna Li Wang, Philip H. Bucksbaum & Zhirong Huang

  11. Argonne National Laboratory, Lemont, IL, USA

    Joseph Z. Xu & Alexander Zholents

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  1. Joseph Duris
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Contributions

A.M. and J.P.C. conceived the experiment, led the experimental team and data analysis and co-wrote the article. J.D. led the electron bunch shaping experimental work and spectral measurement, analysed the spectral data and co-wrote the paper. S.L. designed and built the streaking instrument, participated in the streaking experiment, performed the streaking data analysis and co-wrote the article. T.D. and E.G.C. participated in the streaking experiment, contributed to the streaking data analysis and co-wrote the article. J.P.MacArthur, A.A.L. and Z.Z. participated in the streaking experiment and the electron bunch experimental development, and co-wrote the article. P.R., J.W.A., G.C., J.M.G., G.H., A.K., J.Knurr, J.Krzywinski, M.-F.L., M.N., J.T.O’N., N.S., P.W., A.L.W., T.J.A.W. and M.F.K. participated in the streaking experiment and co-wrote the article. J.Z.X. designed the magnetic wiggler and oversaw the construction of the magnetic wiggler and co-wrote the article. F.-J.D. contributed to the electron bunch shaping development and co-wrote the article. A.Z. helped conceive the experiment and contributed to the design of the magnetic wiggler and co-wrote the article. J.J.W. helped conceive and design the XLEAP beamline and co-wrote the article. Z.H. helped conceive the experiment and design the XLEAP beamline, participated in the electron bunch shaping experiments and co-wrote the article. P.H.B., W.H., A.N. and R.C. helped conceive and participated in the streaking experiment and co-wrote the article. J.P.Marangos helped conceive the experiment and co-wrote the article.

Corresponding authors

Correspondence to James P. Cryan or Agostino Marinelli.

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Supplementary information

Supplementary Information

Beam dynamics, angular streaking set-up, reconstruction algorithm and pulse properties.

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Duris, J., Li, S., Driver, T. et al. Tunable isolated attosecond X-ray pulses with gigawatt peak power from a free-electron laser. Nat. Photonics 14, 30–36 (2020). https://doi.org/10.1038/s41566-019-0549-5

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