Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Article
  • Published:

Generation and measurement of intense few-femtosecond superradiant extreme-ultraviolet free-electron laser pulses

Nature Photonics volume 15, pages 523–529 (2021)Cite this article

Subjects

Abstract

Free-electron lasers producing ultrashort pulses with high peak power promise to extend ultrafast non-linear spectroscopic techniques into the extreme-ultraviolet–X-ray regime. Key aspects are the synchronization between pump and probe, and the control of the pulse properties (duration, intensity and coherence). Externally seeded free-electron lasers produce coherent pulses that can be synchronized with femtosecond accuracy. An important goal is to shorten the pulse duration, but the simple approach of shortening the seed is not sufficient because of the finite-gain bandwidth of the conversion process. An alternative is the amplification of a soliton in a multistage, superradiant cascade: here, we demonstrate the generation of few-femtosecond extreme-ultraviolet pulses, whose duration we measure by autocorrelation. We achieve pulses four times shorter, and with a higher peak power, than in the standard high-gain harmonic generation mode and we prove that the pulse duration matches the Fourier transform limit of the spectral intensity distribution.

This is a preview of subscription content, access via your institution

Access options

Buy this article

  • Purchase on Springer Link
  • Instant access to full article PDF
Buy now

Prices may be subject to local taxes which are calculated during checkout

Fig. 1: FEL layout.
Fig. 2: Pulse duration.
Fig. 3: Pulse energy.
Fig. 4: Pulse spectrum.
Fig. 5: Frequency pulling.

Similar content being viewed by others

Data availability

Source data are provided with this paper. The data that support the plots within this paper and other findings of this study are available from the corresponding author upon reasonable request.

Code availability

The simulation reported in Fig. 4 was carried out with version 2 and version 4 of the code GENESIS 1.3 available at http://genesis.web.psi.ch and https://github.com/svenreiche/Genesis-1.3-Version4.

References

  1. Schreck, S., Beye, M. & Föhlisch, A. Implications of stimulated resonant X-ray scattering for spectroscopy, imaging, and diffraction in the regime from soft to hard X-rays. J. Mod. Opt. 62, S34–S45 (2015).

    Article  ADS  MathSciNet  MATH  Google Scholar 

  2. Calegari, F. et al. Ultrafast electron dynamics in phenylalanine initiated by attosecond pulses. Science 346, 336–339 (2014).

    Article  ADS  Google Scholar 

  3. Berrah, N. A perspective for investigating photo-induced molecular dynamics from within with femtosecond free electron lasers. Phys. Chem. Chem. Phys. 19, 19536–19544 (2017).

    Article  Google Scholar 

  4. Rudenko, A. et al. Femtosecond response of polyatomic molecules to ultra-intense hard X-rays. Nature 546, 129–132 (2017).

    Article  ADS  Google Scholar 

  5. Bencivenga, F., Capotondi, F., Principi, E., Kiskinova, M. & Masciovecchio, C. Coherent and transient states studied with extreme ultraviolet and X-ray free electron lasers: present and future prospects. Adv. Phys. 63, 327–404 (2015).

    Article  ADS  Google Scholar 

  6. Prince, K. C. et al. Coherent control with a short-wavelength free-electron laser. Nat. Photonics 10, 176–179 (2016).

    Article  ADS  Google Scholar 

  7. Danailov, M. B. et al. Towards jitter-free pump-probe measurements at seeded free electron laser facilities. Opt. Express 22, 12869–12879 (2014).

    Article  ADS  Google Scholar 

  8. Allaria, E. et al. Highly coherent and stable pulses from the FERMI seeded free-electron laser in the extreme ultraviolet. Nat. Photonics 6, 699–704 (2012).

    Article  ADS  Google Scholar 

  9. De Ninno, G. et al. Single-shot spectro-temporal characterization of XUV pulses from a seeded free-electron laser. Nat. Commun. 6, 8075 (2015).

    Article  ADS  Google Scholar 

  10. Gorobtsov, O. Y. et al. Seeded X-ray free-electron laser generating radiation with laser statistical properties. Nat. Commun. 9, 4498 (2018).

    Article  ADS  Google Scholar 

  11. Finetti, P. et al. Pulse duration of seeded free-electron lasers. Phys. Rev. X 7, 021043 (2017).

    Google Scholar 

  12. Allaria, E. et al. Two-colour pump–probe experiments with a twin-pulse-seed extreme ultraviolet free-electron laser. Nat. Commun. 4, 2476 (2013).

    Article  ADS  Google Scholar 

  13. McNeil, B. W. J., Thompson, N. R., Dunning, D. J. & Sheehy, B. High harmonic attosecond pulse train amplification in a free electron laser. J. Phys. B 44, 065404 (2011).

    Article  ADS  Google Scholar 

  14. Gauthier, D. et al. Chirped pulse amplification in an extreme-ultraviolet free-electron laser. Nat. Commun. 7, 13688 (2016).

    Article  ADS  Google Scholar 

  15. Tanaka, T. & Rebernic Ribič, P. Shortening the pulse duration in seeded free-electron lasers by chirped microbunching. Opt. Express 27, 30875–30892 (2019).

    Article  ADS  Google Scholar 

  16. Maroju, P. K. et al. Attosecond pulse shaping using a seeded free-electron laser. Nature 578, 386–391 (2020).

    Article  ADS  Google Scholar 

  17. Duris, J. et al. Tunable isolated attosecond X-ray pulses with gigawatt peak power from a free-electron laser. Nat. Photonics 14, 30–36 (2020).

    Article  Google Scholar 

  18. Emma, P. et al. Femtosecond and subfemtosecond X-ray pulses from a self-amplified spontaneous-emission based free-electron laser. Phys. Rev. Lett. 92, 074801 (2004).

    Article  ADS  Google Scholar 

  19. Marinelli, A. et al. Optical shaping of X-ray free-electron lasers. Phys. Rev. Lett. 116, 254801 (2016).

    Article  ADS  Google Scholar 

  20. Behrens, C. et al. Few-femtosecond time-resolved measurements of X-ray free-electron lasers. Nat. Commun. 5, 3762 (2014).

    Article  ADS  Google Scholar 

  21. Ding, Y. et al. Generating femtosecond X-ray pulses using an emittance-spoiling foil in free-electron lasers. Appl. Phys. Lett. 107, 191104 (2015).

    Article  ADS  Google Scholar 

  22. Zholents, A. A. & Penn, G. Obtaining attosecond x-ray pulses using a self-amplified spontaneous emission free electron laser. Phys. Rev. Spec. Top. Accel. Beams 8, 050704 (2005).

    Article  ADS  Google Scholar 

  23. Guetg, M. W. et al. Generation of high-power high-intensity short X-ray free-electron-laser pulses. Phys. Rev. Lett. 120, 014801 (2018).

    Article  ADS  Google Scholar 

  24. Ding, Y. et al. Beam shaping to improve the free-electron laser performance at the Linac Coherent Light Source. Phys. Rev. Accel. Beams 19, 100703 (2016).

    Article  ADS  Google Scholar 

  25. 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).

    Article  ADS  Google Scholar 

  26. 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).

    Article  ADS  Google Scholar 

  27. Giannessi, L., Musumeci, P. & Spampinati, S. Nonlinear pulse evolution in seeded free-electron laser amplifiers and in free-electron laser cascades. J. Appl. Phys. 98, 043110 (2005).

    Article  ADS  Google Scholar 

  28. Bonifacio, R., De Salvo Souza, L., Pierini, P. & Piovella, N. The superradiant regime of a FEL: analytical and numerical results. Nucl. Instrum. Methods Phys. Res. A 296, 358–367 (1990).

    Article  ADS  Google Scholar 

  29. Bonifacio, R., Piovella, N. & McNeil, B. W. J. Superradiant evolution of radiation pulses in a free-electron laser. Phys. Rev. A 44, R3441–R3444 (1991).

    Article  ADS  Google Scholar 

  30. Yang, X., Mirian, N. & Giannessi, L. Postsaturation dynamics and superluminal propagation of a superradiant spike in a free-electron laser amplifier. Phys. Rev. Accel. Beams 23, 010703 (2020).

    Article  ADS  Google Scholar 

  31. Watanabe, T. et al. Experimental characterization of superradiance in a single-pass high-gain laser-seeded free-electron laser amplifier. Phys. Rev. Lett. 98, 034802 (2007).

    Article  ADS  Google Scholar 

  32. Giannessi, L. et al. High-order-harmonic generation and superradiance in a seeded free-electron laser. Phys. Rev. Lett. 108, 164801 (2012).

    Article  ADS  Google Scholar 

  33. Giannessi, L. et al. Superradiant cascade in a seeded free-electron laser. Phys. Rev. Lett. 110, 044801 (2013).

    Article  ADS  Google Scholar 

  34. Svelto, O. & Hanna, D. C. Principles of Lasers (Springer, 2010).

  35. Allaria, E., Ninno, G. D. & Spezzani, C. Experimental demonstration of frequency pulling in single-pass free-electron lasers. Opt. Express 19, 10619–10624 (2011).

    Article  ADS  Google Scholar 

  36. Helml, W. et al. Ultrashort free-electron laser X-ray pulses. Appl. Sci. 7, 915 (2017).

    Article  Google Scholar 

  37. Mitzner, R. et al. Direct autocorrelation of soft-x-ray free-electron-laser pulses by time-resolved two-photon double ionization of He. Phys. Rev. A 80, 025402 (2009).

    Article  ADS  Google Scholar 

  38. Svetina, C. et al. The Low Density Matter (LDM) beamline at FERMI: optical layout and first commissioning. J. Synchrotron Radiat. 22, 538–543 (2015).

    Article  Google Scholar 

  39. Zangrando, M. et al. Recent results of PADReS, the Photon Analysis Delivery and REduction System, from the FERMI FEL commissioning and user operations. J. Synchrotron Radiat. 22, 565–570 (2015).

    Article  Google Scholar 

  40. Reiche, S. GENESIS 1.3: a fully 3D time-dependent FEL simulation code. Nucl. Instrum. Methods Phys. Res. A 429, 243–248 (1999).

    Article  ADS  Google Scholar 

  41. Labat, M. et al. Pulse splitting in short wavelength seeded free electron lasers. Phys. Rev. Lett. 103, 264801 (2009).

    Article  ADS  Google Scholar 

  42. De Ninno, G., Mahieu, B., Allaria, E., Giannessi, L. & Spampinati, S. Chirped seeded free-electron lasers: self-standing light sources for two-color pump-probe experiments. Phys. Rev. Lett. 110, 064801 (2013).

    Article  ADS  Google Scholar 

  43. Mahieu, B. et al. Two-colour generation in a chirped seeded free-electron laser: a close look. Opt. Express 21, 22728–22741 (2013).

    Article  ADS  Google Scholar 

  44. Bonifacio, R., Pellegrini, C. & Narducci, L. M. Collective instabilities and high-gain regime in a free electron laser. Opt. Commun. 50, 373–378 (1984).

    Article  ADS  Google Scholar 

  45. Allaria, E. et al. Two-stage seeded soft-X-ray free-electron laser. Nat. Photonics 7, 913–918 (2013).

    Article  ADS  Google Scholar 

  46. Henke, B. L., Gullikson, E. M. & Davis, J. C. X-ray interactions: photoabsorption, scattering, transmission, and reflection at E = 50–30,000 eV, Z = 1–92. At. Data Nucl. Data Tables 54, 181–342 (1993).

    Article  ADS  Google Scholar 

  47. Düsterer, S. et al. Development of experimental techniques for the characterization of ultrashort photon pulses of extreme ultraviolet free-electron lasers. Phys. Rev. Spec. Top. Accel. Beams 17, 120702 (2014).

    Article  ADS  Google Scholar 

  48. Roling, S. & Zacharias, H. in Synchrotron Light Sources and Free-Electron Lasers (eds Jaeschke, E. et al.) 891–925 (Springer, 2014).

  49. Eland, J. H. D. et al. Complete two-electron spectra in double photoionization: the rare gases Ar, Kr, and Xe. Phys. Rev. Lett. 90, 053003 (2003).

    Article  ADS  Google Scholar 

  50. Squibb, R. J. et al. Acetylacetone photodynamics at a seeded free-electron laser. Nat. Commun. 9, 63 (2018).

    Article  ADS  Google Scholar 

Download references

Acknowledgements

We acknowledge S. Reiche for helpful discussions on bandwidth issues in the simulation of a multistage cascade in GENESIS 1.3. We are also grateful to the whole FERMI team for the dedicated work and support during this experiment.

Author information

Authors and Affiliations

  1. Elettra - Sincrotrone Trieste, Trieste, Italy

    Najmeh S. Mirian, Michele Di Fraia, Simone Spampinati, Filippo Sottocorona, Enrico Allaria, Laura Badano, Miltcho B. Danailov, Alexander Demidovich, Giovanni De Ninno, Simone Di Mitri, Giuseppe Penco, Primož Rebernik Ribič, Carlo Spezzani, Giulio Gaio, Mauro Trovó, Nicola Mahne, Michele Manfredda, Lorenzo Raimondi, Marco Zangrando, Oksana Plekan, Kevin C. Prince, Carlo Callegari & Luca Giannessi

  2. Deutsches Elektronen-Synchrotron DESY, Hamburg, Germany

    Najmeh S. Mirian & Enrico Allaria

  3. Università degli Studi di Trieste, Trieste, Italy

    Filippo Sottocorona

  4. Laboratory of Quantum Optics, University of Nova Gorica, Nova Gorica, Slovenia

    Giovanni De Ninno & Primož Rebernik Ribič

  5. Istituto Officina dei Materiali IOM-CNR, Trieste, Italy

    Marco Zangrando

  6. Centre for Translational Atomaterials, Swinburne University of Technology, Melbourne, Victoria, Australia

    Kevin C. Prince

  7. European XFEL, Schenefeld, Germany

    Tommaso Mazza

  8. University of Gothenburg, Gothenburg, Sweden

    Richard J. Squibb

  9. National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, NY, USA

    Xi Yang

  10. Istituto Nazionale di Fisica Nucleare, Laboratori Nazionali di Frascati, Frascati, Italy

    Luca Giannessi

Authors
  1. Najmeh S. Mirian
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Michele Di Fraia
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Simone Spampinati
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Filippo Sottocorona
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Enrico Allaria
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Laura Badano
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Miltcho B. Danailov
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Alexander Demidovich
    View author publications

    You can also search for this author in PubMed Google Scholar

  9. Giovanni De Ninno
    View author publications

    You can also search for this author in PubMed Google Scholar

  10. Simone Di Mitri
    View author publications

    You can also search for this author in PubMed Google Scholar

  11. Giuseppe Penco
    View author publications

    You can also search for this author in PubMed Google Scholar

  12. Primož Rebernik Ribič
    View author publications

    You can also search for this author in PubMed Google Scholar

  13. Carlo Spezzani
    View author publications

    You can also search for this author in PubMed Google Scholar

  14. Giulio Gaio
    View author publications

    You can also search for this author in PubMed Google Scholar

  15. Mauro Trovó
    View author publications

    You can also search for this author in PubMed Google Scholar

  16. Nicola Mahne
    View author publications

    You can also search for this author in PubMed Google Scholar

  17. Michele Manfredda
    View author publications

    You can also search for this author in PubMed Google Scholar

  18. Lorenzo Raimondi
    View author publications

    You can also search for this author in PubMed Google Scholar

  19. Marco Zangrando
    View author publications

    You can also search for this author in PubMed Google Scholar

  20. Oksana Plekan
    View author publications

    You can also search for this author in PubMed Google Scholar

  21. Kevin C. Prince
    View author publications

    You can also search for this author in PubMed Google Scholar

  22. Tommaso Mazza
    View author publications

    You can also search for this author in PubMed Google Scholar

  23. Richard J. Squibb
    View author publications

    You can also search for this author in PubMed Google Scholar

  24. Carlo Callegari
    View author publications

    You can also search for this author in PubMed Google Scholar

  25. Xi Yang
    View author publications

    You can also search for this author in PubMed Google Scholar

  26. Luca Giannessi
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

N.S.M., S.S. and L.G. conceived the idea of the experiment. C.C. and T.M. conceived the ATI autocorrelation measurement scheme. N.S.M., S.S., E.A., L.B., G.D.N., S.D.M., G.P., P.R., C.S., G.G., M.T., X.Y. and L.G. contributed to the machine operation and tuning for the experiment. S.S., N.S.M. and F.S. simulated the FEL SRC dynamics in the experimental conditions. S.S. and F.S. investigated the energy detuning and the frequency-pulling effect. M.B.D. and A.D. tuned the seed laser for short-pulse operation. N.M., M.M., L.R. and M.Z. designed, aligned and operated the split-and-delay line; O.P., K.C.P., T.M., M.D.F., R.J.S. and C.C. operated the magnetic bottle electron spectrometer, acquired and analysed the cross-correlation data. T.M. and M.D.F. developed the analysis tools used during beam time. N.S.M., C.C., K.C.P. and L.G. wrote the manuscript, which was discussed and agreed by all the coauthors.

Corresponding author

Correspondence to Luca Giannessi.

Ethics declarations

Competing interests

The authors declare no competing interests.

Additional information

Peer review information Nature Photonics thanks Agostino Marinelli and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Supplementary Information

Supplementary Figs. 1–4, Discussion and references.

Source data

Source Data Fig. 2

Data file after analysis for Fig. 2.

Source Data Fig. 3

Data file after analysis for Fig. 3.

Source Data Fig. 4

Data file after analysis for Fig. 4.

Source Data Fig. 5

Zip file containing 7 + 7 HDF5 datasets of acquisitions of the FEL+linac parameters in SRC and HGHG configurations (Fig. 5a and Fig. 5b). Each file corresponds to a different tuning of the resonance in the final amplifier in the two configurations, SRC (Fig. 5a) and HGHG (Fig. 5b). The spectral raw data, to be averaged to prepare the figures, are in the folder /real time/spectrometer PRESTO/GetSpectrum. Each HDF5 file contains all the linac/undulator/beam data from a machine snapshot taken before the acquisition.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Mirian, N.S., Di Fraia, M., Spampinati, S. et al. Generation and measurement of intense few-femtosecond superradiant extreme-ultraviolet free-electron laser pulses. Nat. Photon. 15, 523–529 (2021). https://doi.org/10.1038/s41566-021-00815-w

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41566-021-00815-w

This article is cited by

Search

Advanced search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing