- Physical Review Journals
All JournalsPhysics Magazine

Physical Review Research

Reuse & Permissions

It is not necessary to obtain permission to reuse this article or its components as it is available under the terms of the Creative Commons Attribution 4.0 International license. This license permits unrestricted use, distribution, and reproduction in any medium, provided attribution to the author(s) and the published article's title, journal citation, and DOI are maintained. Please note that some figures may have been included with permission from other third parties. It is your responsibility to obtain the proper permission from the rights holder directly for these figures.

Export citation

Export citation

Choose format for download:

Download Citation
  • Open Access

Generation of isolated white-light attosecond pulses in solids

Gefei Li1,2, Hao Teng1,2,3,*, Zhiyi Wei1,2,3,†, Sheng Meng1,2,3, and Pengju Zhang1,2,3,‡

  • *Contact author: hteng@iphy.ac.cn
  • †Contact author: zywei@iphy.ac.cn
  • ‡Contact author: pengju.zhang@iphy.ac.cn
PDF

Phys. Rev. Research 8, 013067 – Published 22 January, 2026

DOI: https://doi.org/10.1103/8x1z-3l7k

Abstract

Attosecond-pump attosecond-probe spectroscopy (APAP) is the key to understanding electronic-dominated dynamics in light-matter interactions. Although the feasibility of APAP has been demonstrated using isolated attosecond pulses (IAPs), the efforts are mainly confined to the ionization-induced dynamics triggered by the extreme ultraviolet and soft x-ray lights. However, the generation of IAPs capable of exciting neutral electronic excited states, which are more prevalent in nature, is still in its infancy, significantly limiting comprehensive insights into valence-electron wave packet dynamics. Here, we theoretically demonstrate a scheme for the straightforward and compact generation of white-light IAPs covering the visible and ultraviolet regions, based on solid-state high-harmonic generation. By analyzing the strong-field-induced electron-hole dynamics together with a saddle-point approximation, we unfold its microscopic generation mechanism. Furthermore, the feasibility and robustness of this approach are validated by the generation of IAPs from various materials under the same mechanism. Our work paves the way for generation of tabletop white-light IAP sources, thereby harnessing the widespread applications of APAP.

View figure in article

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (73)

  1. P. M. Paul, E. S. Toma, P. Breger, G. Mullot, F. Auge, P. Balcou, H. G. Muller, and P. Agostini, Observation of a train of attosecond pulses from high harmonic generation, Science 292, 1689 (2001).
  2. M. Hentschel, R. Kienberger, C. Spielmann, G. A. Reider, N. Milosevic, T. Brabec, P. Corkum, U. Heinzmann, M. Drescher, and F. Krausz, Attosecond metrology, Nature (London) 414, 509 (2001).
  3. M. Schultze, M. Fieß, N. Karpowicz, J. Gagnon, M. Korbman, M. Hofstetter, S. Neppl, A. L. Cavalieri, Y. Komninos, T. Mercouris, et al., Delay in photoemission, Science 328, 1658 (2010).
  4. K. Klünder, J. M. Dahlström, M. Gisselbrecht, T. Fordell, M. Swoboda, D. Guénot, P. Johnsson, J. Caillat, J. Mauritsson, A. Maquet, R. Taïeb, and A. L’Huillier, Probing single-photon ionization on the attosecond time scale, Phys. Rev. Lett. 106, 143002 (2011).
  5. M. Isinger, R. J. Squibb, D. Busto, S. Zhong, A. Harth, D. Kroon, S. Nandi, C. L. Arnold, M. Miranda, J. M. Dahlström, E. Lindroth, R. Feifel, M. Gisselbrecht, and A. L’Huillier, Photoionization in the time and frequency domain, Science 358, 893 (2017).
  6. G. Schmid, K. Schnorr, S. Augustin, S. Meister, H. Lindenblatt, F. Trost, Y. Liu, N. Stojanovic, A. Al-Shemmary, T. Golz, R. Treusch, M. Gensch, M. Kübel, L. Foucar, A. Rudenko, J. Ullrich, C. D. Schröter, T. Pfeifer, and R. Moshammer, Terahertz-field-induced time shifts in atomic photoemission, Phys. Rev. Lett. 122, 073001 (2019).
  7. M. Huppert, I. Jordan, D. Baykusheva, A. von Conta, and H. J. Wörner, Attosecond delays in molecular photoionization, Phys. Rev. Lett. 117, 093001 (2016).
  8. X. Gong, S. Heck, D. Jelovina, C. Perry, K. Zinchenko, R. Lucchese, and H. J. Wörner, Attosecond spectroscopy of size-resolved water clusters, Nature (London) 609, 507 (2022).
  9. S. Heck, M. Han, D. Jelovina, J.-B. Ji, C. Perry, X. Gong, R. Lucchese, K. Ueda, and H. J. Wörner, Two-center interference in the photoionization delays of Kr2, Phys. Rev. Lett. 129, 133002 (2022).
  10. I. Jordan, M. Huppert, D. Rattenbacher, M. Peper, D. Jelovina, C. Perry, A. von Conta, A. Schild, and H. J. Wörner, Attosecond spectroscopy of liquid water, Science 369, 974 (2020).
  11. S. Li, L. Lu, S. Bhattacharyya, C. Pearce, K. Li, E. T. Nienhuis, G. Doumy, R. D. Schaller, S. Moeller, M.-F. Lin, et al., Attosecond-pump attosecond-probe x-ray spectroscopy of liquid water, Science 383, 1118 (2024).
  12. A. L. Cavalieri, N. Müller, T. Uphues, V. S. Yakovlev, A. Baltuška, B. Horvath, B. Schmidt, L. Blümel, R. Holzwarth, S. Hendel, M. Drescher, U. Kleineberg, P. M. Echenique, R. Kienberger, F. Krausz, and U. Heinzmann, Attosecond spectroscopy in condensed matter, Nature (London) 449, 1029 (2007).
  13. S. Neppl, R. Ernstorfer, E. M. Bothschafter, A. L. Cavalieri, D. Menzel, J. V. Barth, F. Krausz, R. Kienberger, and P. Feulner, Attosecond time-resolved photoemission from core and valence states of magnesium, Phys. Rev. Lett. 109, 087401 (2012).
  14. M. Volkov, S. A. Sato, F. Schlaepfer, L. Kasmi, N. Hartmann, M. Lucchini, L. Gallmann, A. Rubio, and U. Keller, Attosecond screening dynamics mediated by electron localization in transition metals, Nat. Phys. 15, 1145 (2019).
  15. F. Krausz and M. Ivanov, Attosecond physics, Rev. Mod. Phys. 81, 163 (2009).
  16. A. L'Huillier, Nobel lecture: The route to attosecond pulses, Rev. Mod. Phys. 96, 030503 (2024).
  17. F. Martín, F. Calegari, C. Vozzi, K. Ueda, and L. DiMauro, Virtual special issue on attosecond chemistry, J. Phys. Chem. A 128, 4761 (2024).
  18. X. Feng, S. Gilbertson, H. Mashiko, H. Wang, S. D. Khan, M. Chini, Y. Wu, K. Zhao, and Z. Chang, Generation of isolated attosecond pulses with 20 to 28 femtosecond lasers, Phys. Rev. Lett. 103, 183901 (2009).
  19. E. J. Takahashi, P. Lan, O. D. Mücke, Y. Nabekawa, and K. Midorikawa, Infrared two-color multicycle laser field synthesis for generating an intense attosecond pulse, Phys. Rev. Lett. 104, 233901 (2010).
  20. M. Chini, K. Zhao, and Z. Chang, The generation, characterization and applications of broadband isolated attosecond pulses, Nat. Photon. 8, 178 (2014).
  21. T. Gaumnitz, A. Jain, Y. Pertot, M. Huppert, I. Jordan, F. Ardana-Lamas, and H. J. Wörner, Streaking of 43-attosecond soft-X-ray pulses generated by a passively CEP-stable mid-infrared driver, Opt. Express 25, 27506 (2017).
  22. J. Schötz, B. Förg, W. Schweinberger, I. Liontos, H. Masood, A. Kamal, C. Jakubeit, N. Kling, T. Paasch-Colberg, S. Biswas, M. Högner, I. Pupeza, M. Alharbi, A. Azzeer, and M. Kling, Phase-matching for generation of isolated attosecond XUV and soft-X-ray pulses with few-cycle drivers, Phys. Rev. X 10, 041011 (2020).
  23. Y. Yang, R. E. Mainz, G. M. Rossi, F. Scheiba, M. A. Silva-Toledo, P. D. Keathley, G. Cirmi, and F. X. Kärtner, Strong-field coherent control of isolated attosecond pulse generation, Nat. Commun. 12, 6641 (2021).
  24. M. Guan, S. Hu, H. Zhao, C. Lian, and S. Meng, Toward attosecond control of electron dynamics in two-dimensional materials, Appl. Phys. Lett. 116, 043101 (2020).
  25. X.-Y. Wu, H. Liang, X.-S. Kong, Q. Gong, and L.-Y. Peng, Enhancement of high-order harmonic generation in two-dimensional materials by plasmonic fields, Phys. Rev. A 103, 043117 (2021).
  26. Z. Nourbakhsh, N. Tancogne-Dejean, H. Merdji, and A. Rubio, High harmonics and isolated attosecond pulses from MgO, Phys. Rev. Appl. 15, 014013 (2021).
  27. A. Sadeghifaraz, E. Irani, and M. Monfared, Efficient attosecond pulse generation from WS2 semiconductor by tailoring the driving laser pulse, Opt. Commun. 516, 128226 (2022).
  28. P. B. Corkum, Plasma perspective on strong field multiphoton ionization, Phys. Rev. Lett. 71, 1994 (1993).
  29. S. Ghimire, A. D. DiChiara, E. Sistrunk, P. Agostini, L. F. DiMauro, and D. A. Reis, Observation of high-order harmonic generation in a bulk crystal, Nat. Phys. 7, 138 (2011).
  30. G. Vampa, C. McDonald, G. Orlando, D. Klug, P. Corkum, and T. Brabec, Theoretical analysis of high-harmonic generation in solids, Phys. Rev. Lett. 113, 073901 (2014).
  31. M. Wu, D. A. Browne, K. J. Schafer, and M. B. Gaarde, Multilevel perspective on high-order harmonic generation in solids, Phys. Rev. A 94, 063403 (2016).
  32. M. Wu, S. Ghimire, D. A. Reis, K. J. Schafer, and M. B. Gaarde, High-harmonic generation from Bloch electrons in solids, Phys. Rev. A 91, 043839 (2015).
  33. L. Li, P. Lan, X. Zhu, and P. Lu, High harmonic generation in solids: Particle and wave perspectives, Rep. Prog. Phys. 86, 116401 (2023).
  34. See Supplemental Material S2 at http://link.aps.org/supplemental/10.1103/8x1z-3l7k for the description of connection between the dispperion of electron-hole wave packet and the chirp of coherent radiation, which includes Refs. [44, 70].
  35. Z. Chen, M. Levit, Y. Kern, B. Roy, A. Goldner, and M. Krüger, Attosecond pulses from a solid driven by a synthesized two-color field at megahertz repetition rate, ACS Photonics 12, 2819 (2025).
  36. M. Shirozhan, S. Mondal, T. Grósz, B. Nagyillés, B. Farkas, A. Nayak, N. Ahmed, I. Dey, S. C. De Marco, K. Nelissen, et al., High-repetition-rate attosecond extreme ultraviolet beamlines at ELI ALPS for studying ultrafast phenomena, Ultrafast Sci. 4, 0067 (2024).
  37. A. Nayak, D. Rajak, B. Farkas, C. Granados, P. Stammer, J. Rivera-Dean, T. Lamprou, K. Varju, Y. Mairesse, M. F. Ciappina, et al., Attosecond metrology of vacuum-ultraviolet high-order harmonics generated in semiconductors via laser-dressed photoionization of alkali metals, Nat. Commun. 16, 1428 (2025).
  38. S. Ghimire and D. A. Reis, High-harmonic generation from solids, Nat. Phys. 15, 10 (2019).
  39. Á. Jiménez-Galán, R. E. Silva, O. Smirnova, and M. Ivanov, Sub-cycle valleytronics: Control of valley polarization using few-cycle linearly polarized pulses, Optica 8, 277 (2021).
  40. Y.-L. He, J. Guo, F.-Y. Gao, Z.-J. Yang, S.-Q. Zhang, and X.-S. Liu, Interference between harmonics of different crystal momentum channels in solid high-order harmonic generation, Phys. Rev. A 104, 013104 (2021).
  41. See Supplemental Material S13 at http://link.aps.org/supplemental/10.1103/8x1z-3l7k for details on the dynamical evolution of the residual CB population and phase.
  42. T. Higuchi, C. Heide, K. Ullmann, H. B. Weber, and P. Hommelhoff, Light-field-driven currents in graphene, Nature (London) 550, 224 (2017).
  43. M. Du, C. Liu, Y. Zheng, Z. Zeng, and R. Li, Attosecond transient-absorption spectroscopy in one-dimensional periodic crystals, Phys. Rev. A 100, 043840 (2019).
  44. S. A. Oliaei Motlagh, J.-S. Wu, V. Apalkov, and M. I. Stockman, Femtosecond valley polarization and topological resonances in transition metal dichalcogenides, Phys. Rev. B 98, 081406(R) (2018).
  45. See Supplemental Material S9 at http://link.aps.org/supplemental/10.1103/8x1z-3l7k for discussion on the effect of Berry curvature in white-light IAP generation.
  46. A. Bharti, M. Mrudul, and G. Dixit, High-harmonic spectroscopy of light-driven nonlinear anisotropic anomalous Hall effect in a Weyl semimetal, Phys. Rev. B 105, 155140 (2022).
  47. L. Zheng, S. Tang, and X. Chen, Isolated sub-100-as pulse generation by optimizing two-color laser fields using simulated annealing algorithm, Opt. Express 17, 538 (2009).
  48. Y. He, L. He, P. Lan, B. Wang, L. Li, X. Zhu, W. Cao, and P. Lu, Direct imaging of molecular rotation with high-order-harmonic generation, Phys. Rev. A 99, 053419 (2019).
  49. See Supplemental Material S11 at http://link.aps.org/supplemental/10.1103/8x1z-3l7k for the description of simulated annealing.
  50. M. Mrudul, Á. Jiménez-Galán, M. Ivanov, and G. Dixit, Light-induced valleytronics in pristine graphene, Optica 8, 422 (2021).
  51. See Supplemental Material S4 at http://link.aps.org/supplemental/10.1103/8x1z-3l7k for details on derivations of interband current, which includes Refs. [71, 72].
  52. See Supplemental Material S10 at http://link.aps.org/supplemental/10.1103/8x1z-3l7k for discussion on the effect of dephasing time.
  53. N. Rana, M. Mrudul, and G. Dixit, Generation of circularly polarized high harmonics with identical helicity in two-dimensional materials, Phys. Rev. Appl. 18, 064049 (2022).
  54. R. Rajpoot, A. R. Holkundkar, N. Rana, and G. Dixit, Tailoring polarisation of attosecond pulses via co-rotating bicircular laser fields, Phys. Lett. A 493, 129241 (2024).
  55. M. Fanciulli, H. Volfová, S. Muff, J. Braun, H. Ebert, J. Minár, U. Heinzmann, and J. H. Dil, Spin polarization and attosecond time delay in photoemission from spin degenerate states of solids, Phys. Rev. Lett. 118, 067402 (2017).
  56. D. Bauer and K. K. Hansen, High-harmonic generation in solids with and without topological edge states, Phys. Rev. Lett. 120, 177401 (2018).
  57. See Supplemental Material Table S1 at http://link.aps.org/supplemental/10.1103/8x1z-3l7k for the detailed laser parameters used to generate white-light IAP.
  58. O. Melchert, B. Roth, U. Morgner, and A. Demircan, OptFROG—Analytic signal spectrograms with optimized time–frequency resolution, SoftwareX 10, 100275 (2019).
  59. K. Uchida, S. Kusaba, K. Nagai, T. N. Ikeda, and K. Tanaka, Diabatic and adiabatic transitions between Floquet states imprinted in coherent exciton emission in monolayer WSe2, Sci. Adv. 8, eabq7281 (2022).
  60. M. S. Wismer, S. Y. Kruchinin, M. Ciappina, M. I. Stockman, and V. S. Yakovlev, Strong-field resonant dynamics in semiconductors, Phys. Rev. Lett. 116, 197401 (2016).
  61. See Supplemental Material S12 at http://link.aps.org/supplemental/10.1103/8x1z-3l7k for dicussion on the multiphoton excitation pattern under GP and TP excitation conditions.
  62. See Supplemental Material S8 at http://link.aps.org/supplemental/10.1103/8x1z-3l7k for details on derivation about saddle-point method and results.
  63. See Supplemental Material S6 at http://link.aps.org/supplemental/10.1103/8x1z-3l7k for detailed description of IAP temporal profile generated from different materials and corresponding driven laser parameters and materials’ model.
  64. O. Ivakhnenko, S. Shevchenko, and F. Nori, Quantum control via Landau–Zener–Stückelberg–Majorana transitions, Phys. Rep. 995, 1 (2023).
  65. See Supplemental Material S14 at http://link.aps.org/supplemental/10.1103/8x1z-3l7k for details on derivation and plots for strong field resonance parameter and their relation with driving pulse parameters, which includes Ref. [73].
  66. See Supplemental Material Table S5 at http://link.aps.org/supplemental/10.1103/8x1z-3l7k for details on long-pulse duration driven pulse parameter.
  67. C. Manzoni, O. D. Mücke, G. Cirmi, S. Fang, J. Moses, S.-W. Huang, K.-H. Hong, G. Cerullo, and F. X. Kärtner, Coherent pulse synthesis: Towards sub-cycle optical waveforms, Laser Photonics Rev. 9, 129 (2015).
  68. H. J. Wörner, C. A. Arrell, N. Banerji, A. Cannizzo, M. Chergui, A. K. Das, P. Hamm, U. Keller, P. M. Kraus, E. Liberatore, et al., Charge migration and charge transfer in molecular systems, Struct. Dyn. 4, 061508 (2017).
  69. I. C. D. Merritt, D. Jacquemin, and M. Vacher, Attochemistry: Is controlling electrons the future of photochemistry? J. Phys. Chem. Lett. 12, 8404 (2021).
  70. W. Houston, Acceleration of electrons in a crystal lattice, Phys. Rev. 57, 184 (1940).
  71. C. Liu, Y. Zheng, Z. Zeng, and R. Li, Driving-laser ellipticity dependence of high-order harmonic generation in graphene, Phys. Rev. A 97, 063412 (2018).
  72. D. Dimitrovski, T. G. Pedersen, and L. B. Madsen, Floquet-Bloch shifts in two-band semiconductors interacting with light, Phys. Rev. A 95, 063420 (2017).
  73. C. Heide, T. Boolakee, T. Higuchi, and P. Hommelhoff, Adiabaticity parameters for the categorization of light-matter interaction: From weak to strong driving, Phys. Rev. A 104, 023103 (2021).

Outline

Information

Phys. Rev. Research 8, 013067– Published 22 January, 2026
  • Received 28 March 2025
  • Revised 15 September 2025
  • Accepted 22 December 2025
Crossmark - Check for updates button
Creative Commons Logo

Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

Published by the American Physical Society

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation