- Open Access
Single-pass synchronized two-color attosecond x-ray free-electron laser featuring attosecond time jitter
Phys. Rev. Research 8, 023048 – Published 15 April, 2026
DOI: https://doi.org/10.1103/cw2t-yvwd
Abstract
Two-color attosecond x-ray pulses are the key to advancing the study of ultrafast dynamics in quantum systems. In this work, we propose a single-pass free-electron laser scheme generating synchronized attosecond two-color x-ray pulses with femtosecond separation and tens-of-gigawatts peak power. By modulating a chirped electron beam with an infrared laser, we create a periodic train of ultrashort current spikes. This scheme utilizes the limited gain bandwidth of the free-electron laser as a filter, allowing only two adjacent current spikes with different resonance wavelengths to lase. This scheme holds promise for delivering sub-300-as two-color x-ray pulses with an intrinsic timing jitter below 100 as. This work provides insights and technical support for generating two-color attosecond x-ray free-electron laser pulses with robust time jitter.
Physics Subject Headings (PhySH)
Article Text
References (56)
- L. Young et al., Roadmap of ultrafast x-ray atomic and molecular physics, J. Phys. B: At. Mol. Opt. Phys. 51, 032003 (2018).
- A. H. Zewail, Laser femtochemistry, Science 242, 1645 (1988).
- M. Hentschel, R. Kienberger, C. Spielmann, G. A. Reider, N. D. Milovsevic, T. Brabec, P. B. Corkum, U. Heinzmann, M. Drescher, and F. Krausz, Attosecond metrology, Nature (London) 414, 509 (2001).
- E. Takahashi, P. Lan, O. Mücke, and Y. Nabekawa, Attosecond nonlinear optics using gigawatt-scale isolated attosecond pulses, Nat. Commun. 4, 2691 (2013).
- D. Fabris, T. Witting, W. Okell, D. Walke, P. Matia-Hernando, J. Henkel, T. Barillot, M. Lein, J. Marangos, and J. Tisch, Synchronized pulses generated at 20 eV and 90 eV for attosecond pump–probe experiments, Nat. Photon. 9, 383 (2015).
- J. Seres, E. Seres, A. J. Verhoef, G. Tempea, C. Streli, P. Wobrauschek, V. Yakovlev, A. Scrinzi, C. Spielmann, and F. Krausz, Source of coherent kiloelectronvolt X-rays, Nature (London) 433, 596 (2005).
- T. Popmintchev et al., Bright coherent ultrahigh harmonics in the keV x-ray regime from mid-infrared femtosecond lasers, Science 336, 1287 (2012).
- B. Schütte, P. Weber, K. Kovacs, E. Balogh, B. Major, V. Tosa, S. Han, M. Vrakking, K. Varjú, and A. Rouzée, Bright attosecond soft X-ray pulse trains by transient phase-matching in two-color high-order harmonic generation, Opt. Express 23, 33947 (2015).
- P. Emma et al., First lasing and operation of an ångstrom-wavelength free-electron laser, Nat. Photon. 4, 641 (2010).
- T. Ishikawa et al., A compact X-ray free-electron laser emitting in the sub-ångstrom region, Nat. Photon. 6, 540 (2012).
- E. Allaria et al., Two-stage seeded soft-X-ray free-electron laser, Nat. Photon. 7, 913 (2013).
- H.-S. Kang et al., Hard X-ray free-electron laser with femtosecond-scale timing jitter, Nat. Photon. 11, 708 (2017).
- W. Decking et al., A MHz-repetition-rate hard X-ray free-electron laser driven by a superconducting linear accelerator, Nat. Photonics 14, 391 (2020).
- C. J. Milne et al., SwissFEL: The Swiss X-ray Free Electron Laser, Appl. Sci. 7, 720 (2017).
- C. Pellegrini, A. Marinelli, and S. Reiche, The physics of x-ray free-electron lasers, Rev. Mod. Phys. 88, 015006 (2016).
- C. Bostedt, S. Boutet, D. M. Fritz, Z. Huang, H. J. Lee, H. T. Lemke, A. Robert, W. F. Schlotter, J. J. Turner, and G. J. Williams, Linac Coherent Light Source: The first five years, Rev. Mod. Phys. 88, 015007 (2016).
- D. Jaroszynski, R. Prazeres, F. Glotin, and J. Ortega, Two-color free-electron laser operation, Phys. Rev. Lett. 72, 2387 (1994).
- Y. K. Wu, J. Yan, H. Hao, J. Y. Li, S. F. Mikhailov, V. G. Popov, N. A. Vinokurov, S. Huang, and J. Wu, Widely tunable two-color free-electron laser on a storage ring, Phys. Rev. Lett. 115, 184801 (2015).
- A. A. Lutman, R. Coffee, Y. Ding, Z. Huang, J. Krzywinski, T. Maxwell, M. Messerschmidt, and H.-D. Nuhn, Experimental demonstration of femtosecond two-color x-ray free-electron lasers, Phys. Rev. Lett. 110, 134801 (2013).
- T. Hara, Y. Inubushi, T. Katayama, T. Sato, H. Tanaka, T. Tanaka, T. Togashi, K. Togawa, K. Tono, M. Yabashi, and T. Ishikawa, Two-colour hard X-ray free-electron laser with wide tunability, Nat. Commun. 4, 2919 (2013).
- E. Prat, P. Dijkstal, E. Ferrari, R. Ganter, P. Juranić, A. Malyzhenkov, S. Reiche, T. Schietinger, G. Wang, A. A. Haddad, S. Augustin, C. Bostedt, G. Knopp, J. Knurr, A. S. Morillo-Candas, Z. Sun, and K. Schnorr, Widely tunable two-color x-ray free-electron laser pulses, Phys. Rev. Res. 4, L022025 (2022).
- S. Reiche and E. Prat, Two-color operation of a free-electron laser with a tilted beam, J. Synchrotron Radiat. 23, 869 (2016).
- A. A. Lutman, T. J. Maxwell, J. P. MacArthur, M. W. Guetg, N. Berrah, R. N. Coffee, Y. Ding, Z. Huang, A. Marinelli, S. Moeller, and J. C. U. Zemella, Fresh-slice multicolour X-ray free-electron lasers, Nat. Photon. 10, 745 (2016).
- M. W. Guetg, A. A. Lutman, Y. Ding, T. J. Maxwell, and Z. Huang, Dispersion-based fresh-slice scheme for free-electron lasers, Phys. Rev. Lett. 120, 264802 (2018).
- W. Qin, Y. Ding, A. A. Lutman, and Y.-C. Chao, Matching-based fresh-slice method for generating two-color x-ray free-electron lasers, Phys. Rev. Accel. Beams 20, 090701 (2017).
- Y.-C. Chao, W. Qin, Y. Ding, A. A. Lutman, and T. Maxwell, Control of the lasing slice by transverse mismatch in an x-ray free-electron laser, Phys. Rev. Lett. 121, 064802 (2018).
- T. Liu, K. Zhang, Z. Qi, S. Chen, C. Feng, H. Deng, B. Liu, and D. Wang, Matching-based two-color X-ray free-electron laser generation utilizing laser–plasma accelerated electron beam, High Power Laser Sci. Eng. 10, e1 (2022).
- G. Dattoli, N. S. Mirian, E. DiPalma, and V. Petrillo, Two-color free-electron laser with two orthogonal undulators, Phys. Rev. ST Accel. Beams 17, 050702 (2014).
- A. A. Lutman et al., Polarization control in an X-ray free-electron laser, Nat. Photon. 10, 468 (2016).
- J. Duris et al., Tunable isolated attosecond X-ray pulses with gigawatt peak power from a free-electron laser, Nat. Photon. 14, 30 (2020).
- Z. Guo et al., Experimental demonstration of attosecond pump–probe spectroscopy with an X-ray free-electron laser, Nat. Photon. 18, 691 (2024).
- C. Ronsivalle et al., Large-bandwidth two-color free-electron laser driven by a comb-like electron beam, New J. Phys. 16, 033018 (2014).
- A. Marinelli, D. Ratner, A. A. Lutman, J. Turner, J. Welch, F. J. Decker, H. Loos, C. Behrens, S. Gilevich, A. A. Miahnahri, S. Vetter, T. J. Maxwell, Y. Ding, R. Coffee, S. Wakatsuki, and Z. Huang, High-intensity double-pulse X-ray free-electron laser, Nat. Commun. 6, 6369 (2015).
- Y. Ding, C. Behrens, R. Coffee, F.-J. Decker, P. Emma, C. Field, W. Helml, Z. Huang, P. Krejcik, J. Krzywinski, H. Loos, A. Lutman, A. Marinelli, T. J. Maxwell, and J. Turner, Generating femtosecond X-ray pulses using an emittance-spoiling foil in free-electron lasers, Appl. Phys. Lett. 107, 191104 (2015).
- A. Saá Hernández, E. Prat, and S. Reiche, Generation of two-color x-ray free-electron-laser pulses from a beam with a large energy chirp and a slotted foil, Phys. Rev. Accel. Beams 22, 030702 (2019).
- A. Marinelli, R. Coffee, S. Vetter, P. Hering, G. N. West, S. Gilevich, A. A. Lutman, S. Li, T. Maxwell, J. Galayda, A. Fry, and Z. Huang, Optical shaping of x-ray free-electron lasers, Phys. Rev. Lett. 116, 254801 (2016).
- P. Dijkstal, A. Malyzhenkov, S. Reiche, and E. Prat, Demonstration of two-color x-ray free-electron laser pulses with a sextupole magnet, Phys. Rev. Accel. Beams 23, 030703 (2020).
- C. Vicario, S. Bettoni, A. Lutman, A. Dax, M. Huppert, and A. Trisorio, Two-color x-ray free-electron laser by photocathode laser emittance spoiler, Phys. Rev. Accel. Beams 24, 060703 (2021).
- S. Bettoni, P. Craievich, A. Dax, R. Ganter, M. W. Guetg, M. Huppert, F. Marcellini, R. Neto Pestana, S. Reiche, E. Prat, A. Trisorio, C. Vicario, and A. A. Lutman, Experimental demonstration of two-color x-ray free-electron-laser pulses via wakefield excitation, Phys. Rev. Accel. Beams 24, 082801 (2021).
- A. Malyzhenkov, Y. P. Arbelo, P. Craievich, P. Dijkstal, E. Ferrari, S. Reiche, T. Schietinger, P. Juranić, and E. Prat, Single- and two-color attosecond hard x-ray free-electron laser pulses with nonlinear compression, Phys. Rev. Res. 2, 042018 (2020).
- B. Mahieu, E. Allaria, D. Castronovo, M. B. Danailov, A. Demidovich, G. D. Ninno, S. D. Mitri, W. M. Fawley, E. Ferrari, L. Fröhlich, D. Gauthier, L. Giannessi, N. Mahne, G. Penco, L. Raimondi, S. Spampinati, C. Spezzani, C. Svetina, M. Trovò, and M. Zangrando, Two-colour generation in a chirped seeded free-electron laser: A close look, Opt. Express 21, 22728 (2013).
- G. De Ninno, B. Mahieu, E. Allaria, L. Giannessi, and S. Spampinati, Chirped seeded free-electron lasers: Self-standing light sources for two-color pump-probe experiments, Phys. Rev. Lett. 110, 064801 (2013).
- Z. Zhao, H. Li, and Q. Jia, Generation of coherent two-color pulses at two adjacent harmonics in a seeded free-electron laser, Phys. Rev. Accel. Beams 21, 020701 (2018).
- A. A. Lutman, F.-J. Decker, J. Arthur, M. Chollet, Y. Feng, J. Hastings, Z. Huang, H. Lemke, H.-D. Nuhn, A. Marinelli, J. L. Turner, S. Wakatsuki, J. Welch, and D. Zhu, Demonstration of single-crystal self-seeded two-color x-ray free-electron lasers, Phys. Rev. Lett. 113, 254801 (2014).
- S. Roling, S. Braun, P. Gawlitza, M. Wöstmann, E. Ziegler, and H. Zacharias, Tunable two-color hard x-ray multilayer Bragg mirrors, Opt. Lett. 39, 2782 (2014).
- C. Wu, C. Yang, Y. Zhu, K. Hu, Z. Xing, Z. Xu, J. Wu, and W. Zhang, X-ray pulse compressors in Laue diffraction geometry, Opt. Lett. 50, 113 (2025).
- E. Allaria, F. Bencivenga, R. Borghes, F. Capotondi, D. Castronovo, P. Charalambous, P. Cinquegrana, M. Danailov, G. Ninno, A. Demidovich, S. Di Mitri, B. Diviacco, D. Fausti, W. Fawley, E. Ferrari, L. Fröhlich, D. Gauthier, A. Gessini, L. Giannessi, and M. Zangrando, Two-colour pump-probe experiments with a twin-pulse-seed extreme ultraviolet free-electron laser, Nat. Commun. 4, 2476 (2013).
- E. Ferrari, C. Spezzani, F. Fortuna, R. Delaunay, F. Vidal, I. Nikolov, P. Cinquegrana, B. Diviacco, D. Gauthier, G. Penco, P. Ribič, E. Roussel, M. Trovò, J.-B. Moussy, T. Pincelli, L. Lounis, M. Manfredda, E. Pedersoli, F. Capotondi, and M. Sacchi, Widely tunable two-colour seeded free-electron laser source for resonant-pump resonant-probe magnetic scattering, Nat. Commun. 7, 10343 (2016).
- J. P. MacArthur, J. Duris, Z. Zhang, A. Lutman, A. Zholents, X. Xu, Z. Huang, and A. Marinelli, Phase-stable self-modulation of an electron beam in a magnetic wiggler, Phys. Rev. Lett. 123, 214801 (2019).
- S. Reiche, Genesis 1.3: A fully 3D time-dependent fel simulation code, Nucl. Instrum. Methods Phys. Res., Sect. A 429, 243 (1999).
- J. Yan, W. Qin, Y. Chen, W. Decking, P. Dijkstal, M. Guetg, I. Inoue, N. Kujala, S. Liu, T. Long, N. Mirian, and G. Geloni, Terawatt-attosecond hard X-ray free-electron laser at high repetition rate, Nat. Photon. 18, 1293 (2024).
- F. Löhl, V. Arsov, M. Felber, K. Hacker, W. Jalmuzna, B. Lorbeer, F. Ludwig, K.-H. Matthiesen, H. Schlarb, B. Schmidt, P. Schmüser, S. Schulz, J. Szewinski, A. Winter, and J. Zemella, Electron bunch timing with femtosecond precision in a superconducting free-electron laser, Phys. Rev. Lett. 104, 144801 (2010).
- M. Harmand, R. Coffee, M. R. Bionta, M. Chollet, D. French, D. Zhu, D. M. Fritz, H. T. Lemke, N. Medvedev, B. Ziaja, S. Toleikis, and M. Cammarata, Achieving few-femtosecond time-sorting at hard X-ray free-electron lasers, Nat. Photon. 7, 215 (2013).
- T. Sato et al., Femtosecond timing synchronization at megahertz repetition rates for an x-ray free-electron laser, Optica 7, 716 (2020).
- S. Bratos, M. Wulff, and J.-C. Leicknam, XFEL experiments: Jitter of pump–probe time delays and pulse intensities, J. Synchrotron Radiat. 25, 650 (2018).
- S. Bratos and J.-C. Leicknam, Jitter of pump-probe time delays in xfel experiments: How to eliminate it? Chem. Phys. Lett. 754, 137720 (2020).