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.
Subscribe to Journal
Get full journal access for 1 year
only $15.58 per issue
All prices are NET prices.
VAT will be added later in the checkout.
Rent or Buy article
Get time limited or full article access on ReadCube.
All prices are NET prices.
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.
Hentschel, M. et al. Attosecond metrology. Nature 414, 509–513 (2001).
Li, X. F. et al. Multiple-harmonic generation in rare gases at high laser intensity. Phys. Rev. A 39, 5751–5761 (1989).
Corkum, P. B. & Krausz, F. Attosecond science. Nat. Phys. 3, 381–387 (2007).
Chang, Z. & Corkum, P. Attosecond photon sources: the first decade and beyond [invited]. J. Opt. Soc. Am. B 27, B9–B17 (2010).
Ciappina, M. F. et al. Attosecond physics at the nanoscale. Rep. Prog. Phys. 80, 054401 (2017).
Sekikawa, T., Kosuge, A., Kanai, T. & Watanabe, S. Nonlinear optics in the extreme ultraviolet. Nature 432, 605–608 (2004).
Sansone, G. et al. Isolated single-cycle attosecond pulses. Science 314, 443–446 (2006).
Sola, I. J. et al. Controlling attosecond electron dynamics by phase-stabilized polarization gating. Nat. Phys. 2, 319–322 (2006).
Goulielmakis, E. et al. Single-cycle nonlinear optics. Science 320, 1614–1617 (2008).
Mashiko, H. et al. Double optical gating of high-order harmonic generation with carrier-envelope phase stabilized lasers. Phys. Rev. Lett. 100, 103906 (2008).
Feng, X. et al. Generation of isolated attosecond pulses with 20 to 28 femtosecond lasers. Phys. Rev. Lett. 103, 183901 (2009).
Ferrari, F. et al. High-energy isolated attosecond pulses generated by above-saturation few-cycle fields. Nat. Photon. 4, 875–879 (2010).
Takahashi, E. J., Lan, P., Mcke, O. D., Nabekawa, Y. & Midorikawa, K. Attosecond nonlinear optics using gigawatt-scale isolated attosecond pulses. Nat. Commun. 4, 2691 (2013).
Ossiander, M. et al. Attosecond correlation dynamics. Nat. Phys. 13, 280–285 (2017).
Barillot, T. R. et al. Towards XUV pump-probe experiments in the femtosecond to sub-femtosecond regime: new measurement of the helium two-photon ionization cross-section. Chem. Phys. Lett. 683, 38–42 (2017).
Bergues, B. et al. Tabletop nonlinear optics in the 100-eV spectral region. Optica 5, 237–242 (2018).
Jahn, O. et al. Towards intense isolated attosecond pulses from relativistic surface high harmonics. Optica 6, 280–287 (2019).
Teichmann, S. M., Silva, F., Cousin, S. L., Hemmer, M. & Biegert, J. 0.5-keV soft X-ray attosecond continua. Nat. Commun. 7, 11493 (2016).
Gaumnitz, T. et al. Streaking of 43-attosecond soft-X-ray pulses generated by a passively CEP-stable mid-infrared driver. Opt. Express 25, 27506–27518 (2017).
Li, J. et al. 53-attosecond X-ray pulses reach the carbon K-edge. Nat. Commun. 8, 186 (2017).
Johnson, A. S. et al. High-flux soft x-ray harmonic generation from ionization-shaped few-cycle laser pulses. Sci. Adv. 4, eaar3761 (2018).
Wolf, T. J. A. et al. Probing ultrafast ππ*/nπ* internal conversion in organic chromophores via K-edge resonant absorption. Nat. Commun. 8, 29 (2017).
Neville, S. P., Chergui, M., Stolow, A. & Schuurman, M. S. Ultrafast X-ray spectroscopy of conical intersections. Phys. Rev. Lett. 120, 243001 (2018).
Attar, A. R. et al. Femtosecond x-ray spectroscopy of an electrocyclic ring-opening reaction. Science 356, 54–59 (2017).
Schütte, B. et al. Bright attosecond soft X-ray pulse trains by transient phase-matching in two-color high-order harmonic generation. Opt. Express 23, 33947–33955 (2015).
Leone, S. R. et al. What will it take to observe processes in ’real time’? Nat. Photon. 8, 162–166 (2014).
Lépine, F., Ivanov, M. Y. & Vrakking, M. J. J. Attosecond molecular dynamics: fact or fiction? Nat. Photon. 8, 195–204 (2014).
Ackermann, W. et al. Operation of a free-electron laser from the extreme ultraviolet to the water window. Nat. Photon. 1, 336–342 (2007).
Emma, P. et al. First lasing and operation of an ångstrom-wavelength free-electron laser. Nat. Photon. 4, 641–647 (2010).
Allaria, E. et al. Highly coherent and stable pulses from the FERMI seeded free-electron laser in the extreme ultraviolet. Nat. Photon. 6, 699–704 (2012).
Allaria, E. et al. Two-stage seeded soft-X-ray free-electron laser. Nat. Photon. 7, 913–918 (2013).
Ishikawa, T. et al. A compact X-ray free-electron laser emitting in the sub-ångström region. Nat. Photon. 6, 540–544 (2012).
Kang, H.-S. et al. Hard X-ray free-electron laser with femtosecond-scale timing jitter. Nat. Photon. 11, 708–713 (2017).
Altarelli, M. The European X-ray free-electron laser facility in Hamburg. Nuclear Instrum. Methods Phys. Res. Sect. B 269, 2845–2849 (2011).
Bonifacio, R., Pellegrini, C. & Narducci, L. Collective instabilities and high-gain regime in a free-electron laser. Opt. Commun. 50, 373–378 (1984).
Pellegrini, C., Marinelli, A. & Reiche, S. The physics of x-ray free-electron lasers. Rev. Mod. Phys. 88, 015006 (2016).
Huang, Z. & Kim, K.-J. Review of x-ray free-electron laser theory. Phys. Rev. ST Accel. Beams 10, 034801 (2007).
Bonifacio, R., DeSalvo, L., Pierini, P., Piovella, N. & Pellegrini, C. Spectrum, temporal structure, and fluctuations in a high-gain free-electron laser starting from noise. Phys. Rev. Lett. 73, 70–73 (1994).
Huang, S. et al. Generating single-spike hard x-ray pulses with nonlinear bunch compression in free-electron lasers. Phys. Rev. Lett. 119, 154801 (2017).
Marinelli, A. et al. Experimental demonstration of a single-spike hard-X-ray free-electron laser starting from noise. Appl. Phys. Lett. 111, 151101 (2017).
Behrens, C. et al. Few-femtosecond time-resolved measurements of X-ray free-electron lasers. Nat. Commun. 5, 3762 (2014).
Hartmann, N. et al. Attosecond time–energy structure of X-ray free-electron laser pulses. Nat. Photon. 12, 215–220 (2018).
Zholents, A. A. Method of an enhanced self-amplified spontaneous emission for x-ray free electron lasers. Phys. Rev. ST Accel. Beams 8, 040701 (2005).
MacArthur, J. P. et al. Phase-stable self-modulation of an electron beam in a magnetic wiggler. Phys. Rev. Lett. 123, 214801 (2019).
Li, S. et al. A co-axial velocity map imaging spectrometer for electrons. AIP Adv. 8, 115308 (2018).
Kienberger, R. et al. Atomic transient recorder. Nature 427, 817–821 (2004).
Kazansky, A. K., Bozhevolnov, A. V., Sazhina, I. P. & Kabachnik, N. M. Interference effects in angular streaking with a rotating terahertz field. Phys. Rev. A 93, 013407 (2016).
Kazansky, A. K., Sazhina, I. P., Nosik, V. L. & Kabachnik, N. M. Angular streaking and sideband formation in rotating terahertz and far-infrared fields. J. Phys. B 50, 105601 (2017).
Li, S. et al. Characterizing isolated attosecond pulses with angular streaking. Opt. Express 26, 4531–4547 (2018).
Itatani, J. et al. Attosecond streak camera. Phys. Rev. Lett. 88, 173903 (2002).
Glownia, J. M. et al. Time-resolved pump-probe experiments at the LCLS. Opt. Express 18, 17620–17630 (2010).
Zhang, Z., Duris, J., MacArthur, J. P., Huang, Z. & Marinelli, A. Double chirp-taper x-ray free-electron laser for attosecond pump-probe experiments. Phys. Rev. Accel. Beams 22, 050701 (2019).
Ding, Y., Huang, Z., Ratner, D., Bucksbaum, P. & Merdji, H. Generation of attosecond x-ray pulses with a multicycle two-color enhanced self-amplified spontaneous emission scheme. Phys. Rev. ST Accel. Beams 12, 060703 (2009).
Mukamel, S., Healion, D., Zhang, Y. & Biggs, J. D. Multidimensional attosecond resonant X-ray spectroscopy of molecules: lessons from the optical regime. Annu. Rev. Phys. Chem. 64, 101–127 (2013).
Lutman, A. A. et al. Experimental demonstration of femtosecond two-color x-ray free-electron lasers. Phys. Rev. Lett. 110, 134801 (2013).
Schoenlein, R. et al. New Science Opportunities Enabled by LCLS-II X-ray Lasers SLAC Pub. SLAC-R-1053 https://portal.slac.stanford.edu/sites/lcls_public/Documents/LCLS-IIScienceOpportunities_final.pdf (SLAC National Accelerator Laboratory, 2015).
Marinelli, A. et al. Multicolor operation and spectral control in a gain-modulated X-ray free-electron laser. Phys. Rev. Lett. 111, 134801 (2013).
Schweigert, I. V. & Mukamel, S. Probing valence electronic wave-packet dynamics by all X-ray stimulated Raman spectroscopy: a simulation study. Phys. Rev. A 76, 012504 (2007).
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.
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
About this article
Cite this article
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 (2019) doi:10.1038/s41566-019-0549-5
Attosecond transient absorption spooktroscopy: a ghost imaging approach to ultrafast absorption spectroscopy
Physical Chemistry Chemical Physics (2020)