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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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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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.
The authors declare no competing interests.
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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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