- Open Access
Few-Femtosecond XUV Pulse Pairs with Independently Tunable Topological Properties
Phys. Rev. Lett. 136, 195001 – Published 11 May, 2026
DOI: https://doi.org/10.1103/b2pw-pmxn
Abstract
By leveraging a recently developed slippage-compensation scheme in externally seeded free-electron lasers (FELs), we propose a method for generating few-femtosecond extreme-ultraviolet (XUV) pulse pairs with tunable topological properties and adjustable temporal delay. Simulations show that the topological charge of each pulse can be independently set to , 0, 1, while the delay between the pulses can be tuned from a few to several tens of femtoseconds. Compared with superradiance—the only other currently viable approach for producing XUV pulse pairs with these characteristics—the proposed scheme offers greater flexibility, as it does not require driving the FEL into saturation, which typically necessitates a cascade configuration. Furthermore, when combined with pulse-to-pulse polarization switching, this approach has the potential to extend XUV studies of circular and helical dichroism in chiral systems and magnetic materials, as well as high-resolution imaging, into the few-femtosecond regime.
Physics Subject Headings (PhySH)
Article Text
References (51)
- B. W. J. McNeil and N. R. Thompson, X-ray free-electron lasers, Nat. Photonics 4, 814 (2010).
- N. Huang, H. Deng, B. Liu, D. Wang, and Z. Zhao, Features and futures of X-ray free-electron lasers, Innovation 2, 100097 (2021).
- L. Yu et al., High-gain harmonic-generation free-electron laser, Science 289, 932 (2000).
- D. Gauthier, P. R. Ribič, G. De Ninno, E. Allaria, P. Cinquegrana, M. B. Danailov, A. Demidovich, E. Ferrari, L. Giannessi, B. Mahieu, and G. Penco, Spectrotemporal shaping of seeded free-electron laser pulses, Phys. Rev. Lett. 115, 114801 (2015).
- D. Gauthier, P. R. Ribič, G. De Ninno, E. Allaria, P. Cinquegrana, M. B. Danailov, A. Demidovich, E. Ferrari, and L. Giannessi, Generation of phase-locked pulses from a seeded free-electron laser, Phys. Rev. Lett. 116, 024801 (2016).
- G. Perosa et al., Femtosecond polarization shaping of free-electron laser pulses, Phys. Rev. Lett. 131, 045001 (2023).
- M. Dumergue et al., Wave-packet manipulation of He Rydberg states by a seeded free-electron laser, Phys. Rev. Res. 6, 043323 (2024).
- A. Wituschek et al., Tracking attosecond electronic coherences using phase-manipulated extreme ultraviolet pulses, Nat. Commun. 11, 883 (2020).
- F. Richter et al., Strong-field quantum control in the extreme ultraviolet domain using pulse shaping, Nature (London) 636, 337 (2024).
- J. Bahrdt, K. Holldack, P. Kuske, R. Müller, M. Scheer, and P. Schmid, First observation of photons carrying orbital angular momentum in undulator radiation, Phys. Rev. Lett. 111, 034801 (2013).
- E. Hemsing, A. Knyazik, M. Dunning, D. Xiang, A. Marinelli, C. Hast, and J. Rosenzweig, Coherent optical vortices from relativistic electron beams, Nat. Phys. 9, 549 (2013).
- E. Hemsing, M. Dunning, C. Hast, T. Raubenheimer, and D. Xiang, First characterization of coherent optical vortices from harmonic undulator radiation, Phys. Rev. Lett. 113, 134803 (2014).
- P. Rebernik Ribič, B. Rösner, D. Gauthier, E. Allaria, F. Döring, L. Foglia, L. Giannessi, N. Mahne, M. Manfredda, C. Masciovecchio, R. Mincigrucci, N. Mirian, E. Principi, E. Roussel, A. Simoncig, S. Spampinati, C. David, and G. De Ninno, Extreme-ultraviolet vortices from a free-electron laser, Phys. Rev. X 7, 031036 (2017).
- S. Matsuba, K. Kawase, A. Miyamoto, S. Sasaki, M. Fujimoto, T. Konomi, N. Yamamoto, M. Hosaka, and M. Katoh, Generation of vector beam with tandem helical undulators, Appl. Phys. Lett. 113, 021106 (2018).
- J. Morgan, P. Rebernik Ribič, F. Capotondi, A. Brynes, M. Manfredda, G. De Ninno, L. Novinec, M. Pancaldi, E. Pedersoli, A. Simoncig, C. Spezzani, M. Zangrando, and E. Hemsing, Poincaré beams from a free electron laser, Nat. Photonics 19, 946 (2025).
- M. Fanciulli et al., Observation of magnetic helicoidal dichroism with extreme ultraviolet light vortices, Phys. Rev. Lett. 128, 077401 (2022).
- M. Fanciulli et al., Magnetic vortex dynamics probed by time-resolved magnetic helicoidal dichroism, Phys. Rev. Lett. 134, 156701 (2025).
- A. A. Sirenko, P. Marsik, C. Bernhard, T. N. Stanislavchuk, V. Kiryukhin, and S.-W. Cheong, Terahertz vortex beam as a spectroscopic probe of magnetic excitations, Phys. Rev. Lett. 122, 237401 (2019).
- J. Rouxel, B. Rösner, D. Karpov, C. Bacellar, G. Mancini, F. Zinna, D. Kinschel, O. Cannelli, M. Oppermann, C. Svetina, A. Diaz, J. Lacour, C. David, and M. Chergui, Hard X-ray helical dichroism of disordered molecular media, Nat. Photonics 16, 570 (2022).
- S. Huang, Y. Ding, Y. Feng, E. Hemsing, Z. Huang, J. Krzywinski, A. A. Lutman, A. Marinelli, T. J. Maxwell, and D. Zhu, Generating single-spike hard X-ray pulses with nonlinear bunch compression in free-electron lasers, Phys. Rev. Lett. 119, 154801 (2017).
- J. Duris et al., Tunable isolated attosecond X-ray pulses with gigawatt peak power from a free-electron laser, Nat. Photonics 14, 30 (2020).
- 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(R) (2020).
- 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. Photonics 18, 1293 (2024).
- N. Sudar, R. Coffee, and E. Hemsing, Coherent X rays with tunable time-dependent polarization, Phys. Rev. Accel. Beams 23, 120701 (2020).
- J. Morgan and B. W. J. McNeil, Attosecond polarization modulation of x-ray radiation in a free-electron laser, Phys. Rev. Accel. Beams 24, 010701 (2021).
- J. Morgan and B. W. J. McNeil, X-ray pulse generation with ultra-fast flipping of its orbital angular momentum, Opt. Express 30, 31171 (2022).
- M. Ferray, A. L’Huillier, X. F. Li, L. A. Lompre, G. Mainfray, and C. Manus, Multiple-harmonic conversion of 1064 nm radiation in rare gases, J. Phys. B 21, L31 (1988).
- J. Li, J. Lu, A. Chew, S. Han, J. Li, Y. Wu, H. Wang, S. Ghimire, and Z. Chang, Attosecond science based on high harmonic generation from gases and solids, Nat. Commun. 11, 2748 (2020).
- R. Bonifacio, B. W. J. McNeil, and P. Pierini, Superradiance in the high-gain free-electron laser, Phys. Rev. A 40, 4467 (1989).
- N. S. Mirian et al., Generation and measurement of intense few-femtosecond superradiant extreme-ultraviolet free-electron laser pulses, Nat. Photonics 15, 523 (2021).
- D. Gauthier et al., Chirped pulse amplification in an extreme-ultraviolet free-electron laser, Nat. Commun. 7, 13688 (2016).
- T. Tanaka, Proposal to generate an isolated monocycle x-ray pulse by counteracting the slippage effect in free-electron lasers, Phys. Rev. Lett. 114, 044801 (2015).
- T. Tanaka and P. R. Ribič, Shortening the pulse duration in seeded free-electron lasers by chirped microbunching, Opt. Express 27, 30875 (2019).
- P. R. Ribič and T. Tanaka, Isolated single-cycle extreme-ultraviolet pulses from undulator radiation, Opt. Lett. 45, 5234 (2020).
- S. Sasaki and I. McNulty, Proposal for generating brilliant X-ray beams carrying orbital angular momentum, Phys. Rev. Lett. 100, 124801 (2008).
- L. Allen, M. W. Beijersbergen, R. J. C. Spreeuw, and J. P. Woerdman, Orbital angular momentum of light and the transformation of Laguerre-Gaussian laser modes, Phys. Rev. A 45, 8185 (1992).
- T. Tanaka, SIMPLEX: Simulator and postprocessor for free-electron laser experiments, J. Synchrotron Radiat. 22, 1319 (2015).
- T. Tanaka, Numerical methods for free electron laser simulations, J. Electromagn. Waves Appl. 32, 371 (2018).
- T. Tanaka, Accelerating the convergence of free electron laser simulations by retrieving a spatially coherent component of microbunching, Phys. Rev. Accel. Beams 27, 030703 (2024).
- T. Tanaka, Y. Kida, R. Kinjo, T. Togashi, H. Tomizawa, S. Hashimoto, S. Miyamoto, S. Okabe, and Y. Tanaka, Development of an undulator with a variable magnetic field profile, J. Synchrotron Radiat. 28, 404 (2021).
The slight asymmetry of the OAM mode observed in Fig. 4 indicates a small admixture of additional modes (at the few-percent energy level), consistent with previous studies of OAM generation in undulators (see, e.g., Refs. [13, 42, 43, 44]).
- E. Hemsing, A. Marinelli, and J. B. Rosenzweig, Generating optical orbital angular momentum in a high-gain free-electron laser at the first harmonic, Phys. Rev. Lett. 106, 164803 (2011).
- P. R. Ribič, D. Gauthier, and G. De Ninno, Generation of coherent extreme-ultraviolet radiation carrying orbital angular momentum, Phys. Rev. Lett. 112, 203602 (2014).
- C. Xu, J. Yan, G. Geloni, C. Lechner, and H. Deng, Spatiotemporal shaping of attosecond X-rays with time-dependent orbital angular momentum, arXiv:2508.19020v2.
Undesired harmonics, such as the fundamental in case of Fig. 2, are typically removed using standard spectral filters before reaching the experimental station, as done in Refs. [13, 15]. A variety of filters is available at FEL facilities, and for many experiments, partial filtering is sufficient, particularly when the measurements are energy resolved.
- F. Kong, C. Zhang, F. Bouchard, Z. Li, G. G. Brown, D. H. Ko, T. J. Hammond, L. Arissian, R. W. Boyd, E. Karimi, and P. B. Corkum, Controlling the orbital angular momentum of high harmonic vortices, Nat. Commun. 8, 14970 (2017).
- D. Gauthier, P. R. Ribič, G. Adhikary, A. Camper, C. Chappuis, R. Cucini, L. F. DiMauro, G. Dovillaire, F. Frassetto, R. Géneaux, P. Miotti, L. Poletto, B. Ressel, C. Spezzani, M. Stupar, T. Ruchon, and G. De Ninno, Tunable orbital angular momentum in high-harmonic generation, Nat. Commun. 8, 14971 (2017).
- P. V. Demekhin, A. N. Artemyev, A. Kastner, and T. Baumert, Photoelectron circular dichroism with two overlapping laser pulses of carrier frequencies and linearly polarized in two mutually orthogonal directions, Phys. Rev. Lett. 121, 253201 (2018).
- L. Foglia et al., Nanoscale polarization transient gratings, Nat. Commun. 15, 10742 (2024).
- L. Ye, J. R. Rouxel, S. Asban, B. Rösner, and S. Mukamel, Probing molecular chirality by orbital-angular-momentum-carrying X-ray pulses, J. Chem. Theory Comput. 15, 4180 (2019).
- X. Jiang, Y. Nam, J. R. Rouxel, H. Yong, and S. Mukamel, Time-resolved enantiomer-exchange probed by using the orbital angular momentum of X-ray light, Chem. Sci. 14, 11067 (2023).