- Letter
- Open Access
Chiral electron momentum distribution upon strong-field ionization of atoms
Phys. Rev. Research 7, L032061 – Published 18 September, 2025
DOI: https://doi.org/10.1103/8pnf-fmqt
Abstract
We present a scheme to synthesize a three-dimensional laser field that produces a chiral electron momentum distribution upon strong-field ionization of atoms. Our approach employs two orthogonally propagating two-color laser beams. This results in a time-dependent three-dimensional electric field vector of the combined light field that varies for different positions within the focal volume. For each position, we conduct a simulation of the corresponding electron momentum distribution that includes nonadiabatic dynamics and Coulomb interaction after tunneling. For suitable laser parameters, only a small region of the focal volume contributes to the final momentum distribution. Thus, integrating over all position coordinates, a specific chiral laser field dominates. This leads to a volume-averaged electron momentum distribution, which is chiral, as well. This work will serve as a benchmark for future strong-field experiments aiming at the synthetization of well-defined, three-dimensional laser fields.
Physics Subject Headings (PhySH)
Article Text
References (54)
- L. V. Keldysh, Ionization in the field of a strong electromagnetic wave, Sov. Phys. JETP 20, 1307 (1965).
- P. Agostini, F. Fabre, G. Mainfray, G. Petite, and N. K. Rahman, Free-free transitions following six-photon ionization of xenon atoms, Phys. Rev. Lett. 42, 1127 (1979).
- P. H. Bucksbaum, M. Bashkansky, R. R. Freeman, T. J. McIlrath, and L. F. DiMauro, Suppression of multiphoton ionization with circularly polarized coherent light, Phys. Rev. Lett. 56, 2590 (1986).
- P. B. Corkum, N. H. Burnett, and F. Brunel, Above-threshold ionization in the long-wavelength limit, Phys. Rev. Lett. 62, 1259 (1989).
- J. L. Krause, K. J. Schafer, and K. C. Kulander, High-order harmonic generation from atoms and ions in the high intensity regime, Phys. Rev. Lett. 68, 3535 (1992).
- P. Eckle, A. N. Pfeiffer, C. Cirelli, A. Staudte, R. Dörner, H. G. Muller, M. Büttiker, and U. Keller, Attosecond ionization and tunneling delay time measurements in helium, Science 322, 1525 (2008).
- V. Hanus, S. Kangaparambil, S. Larimian, M. Dorner-Kirchner, X. Xie, M. S. Schöffler, G. G. Paulus, A. Baltuška, A. Staudte, and M. Kitzler-Zeiler, Subfemtosecond tracing of molecular dynamics during strong-field interaction, Phys. Rev. Lett. 123, 263201 (2019).
- M. Meckel, D. Comtois, D. Zeidler, A. Staudte, D. Pavičić, H. C. Bandulet, H. Pépin, J. C. Kieffer, R. Dörner, D. M. Villeneuve, and P. B. Corkum, Laser-induced electron tunneling and diffraction, Science 320, 1478 (2008).
- T. Weber, H. Giessen, M. Weckenbrock, G. Urbasch, A. Staudte, L. Spielberger, O. Jagutzki, V. Mergel, M. Vollmer, and R. Dörner, Correlated electron emission in multiphoton double ionization, Nature (London) 405, 658 (2000).
- A. Staudte, S. Patchkovskii, D. Pavičić, H. Akagi, O. Smirnova, D. Zeidler, M. Meckel, D. M. Villeneuve, R. Dörner, M. Y. Ivanov, and P. B. Corkum, Angular tunneling ionization probability of fixed-in-space molecules in intense laser pulses, Phys. Rev. Lett. 102, 033004 (2009).
- L. Arissian, C. Smeenk, F. Turner, C. Trallero, A. V. Sokolov, D. M. Villeneuve, A. Staudte, and P. B. Corkum, Direct test of laser tunneling with electron momentum imaging, Phys. Rev. Lett. 105, 133002 (2010).
- W. Becker, B. N. Chichkov, and B. Wellegehausen, Schemes for the generation of circularly polarized high-order harmonics by two-color mixing, Phys. Rev. A 60, 1721 (1999).
- C. A. Mancuso, D. D. Hickstein, P. Grychtol, R. Knut, O. Kfir, X.-M. Tong, F. Dollar, D. Zusin, M. Gopalakrishnan, C. Gentry, E. Turgut, J. L. Ellis, M.-C. Chen, A. Fleischer, O. Cohen, H. C. Kapteyn, and M. M. Murnane, Strong-field ionization with two-color circularly polarized laser fields, Phys. Rev. A 91, 031402(R) (2015).
- C. A. Mancuso, K. M. Dorney, D. D. Hickstein, J. L. Chaloupka, X.-M. Tong, J. L. Ellis, H. C. Kapteyn, and M. M. Murnane, Observation of ionization enhancement in two-color circularly polarized laser fields, Phys. Rev. A 96, 023402 (2017).
- A. Fleischer, O. Kfir, T. Diskin, P. Sidorenko, and O. Cohen, Spin angular momentum and tunable polarization in high-harmonic generation, Nat. Photon. 8, 543 (2014).
- I. Barth and O. Smirnova, Nonadiabatic tunneling in circularly polarized laser fields: Physical picture and calculations, Phys. Rev. A 84, 063415 (2011).
- T. Herath, L. Yan, S. K. Lee, and W. Li, Strong-field ionization rate depends on the sign of the magnetic quantum number, Phys. Rev. Lett. 109, 043004 (2012).
- I. Barth and O. Smirnova, Spin-polarized electrons produced by strong-field ionization, Phys. Rev. A 88, 013401 (2013).
- S. Eckart, K. Fehre, N. Eicke, A. Hartung, J. Rist, D. Trabert, N. Strenger, A. Pier, L. Ph. H. Schmidt, T. Jahnke, M. S. Schöffler, M. Lein, M. Kunitski, and R. Dörner, Direct experimental access to the nonadiabatic initial momentum offset upon tunnel ionization, Phys. Rev. Lett. 121, 163202 (2018).
- S. Eckart, M. Kunitski, M. Richter, A. Hartung, J. Rist, F. Trinter, K. Fehre, N. Schlott, K. Henrichs, L. Ph. H. Schmidt, T. Jahnke, M. Schöffler, K. Liu, I. Barth, J. Kaushal, F. Morales, M. Ivanov, O. Smirnova, and R. Dörner, Ultrafast preparation and detection of ring currents in single atoms, Nat. Phys. 14, 701 (2018).
- D. Trabert, S. Brennecke, K. Fehre, N. Anders, A. Geyer, S. Grundmann, M. Schöffler, L. Ph. H. Schmidt, T. Jahnke, R. Dörner, M. Kunitski, and S. Eckart, Angular dependence of the Wigner time delay upon tunnel ionization of , Nat. Commun. 12, 1697 (2021).
- M. Han, P. Ge, Y. Shao, Q. Gong, and Y. Liu, Attoclock photoelectron interferometry with two-color corotating circular fields to probe the phase and the amplitude of emitting wave packets, Phys. Rev. Lett. 120, 073202 (2018).
- R. Murray, W.-K. Liu, and M. Y. Ivanov, Partial Fourier-transform approach to tunnel ionization: Atomic systems, Phys. Rev. A 81, 023413 (2010).
- 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).
- 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. Photon. 13, 866 (2019).
- O. Neufeld, D. Ayuso, P. Decleva, M. Y. Ivanov, O. Smirnova, and O. Cohen, Ultrasensitive chiral spectroscopy by dynamical symmetry breaking in high harmonic generation, Phys. Rev. X 9, 031002 (2019).
- O. Neufeld, M. Even Tzur, and O. Cohen, Degree of chirality of electromagnetic fields and maximally chiral light, Phys. Rev. A 101, 053831 (2020).
- N. Mayer, S. Patchkovskii, F. Morales, M. Ivanov, and O. Smirnova, Imprinting chirality on atoms using synthetic chiral light fields, Phys. Rev. Lett. 129, 243201 (2022).
- N. Mayer, D. Ayuso, P. Decleva, M. Khokhlova, E. Pisanty, M. Ivanov, and O. Smirnova, Chiral topological light for detection of robust enantiosensitive observables, Nat. Photon. 18, 1155 (2024).
- 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).
- L. Rego and D. Ayuso, Structuring the local handedness of synthetic chiral light: Global chirality versus polarization of chirality, New J. Phys. 25, 093005 (2023).
- P. B. Corkum, Plasma perspective on strong field multiphoton ionization, Phys. Rev. Lett. 71, 1994 (1993).
- N. I. Shvetsov-Shilovski, M. Lein, L. B. Madsen, E. Räsänen, C. Lemell, J. Burgdörfer, D. G. Arbó, and K. Tőkési, Semiclassical two-step model for strong-field ionization, Phys. Rev. A 94, 013415 (2016).
- H. Ni, U. Saalmann, and J.-M. Rost, Tunneling exit characteristics from classical backpropagation of an ionized electron wave packet, Phys. Rev. A 97, 013426 (2018).
- S. Brennecke, N. Eicke, and M. Lein, Gouy's phase anomaly in electron waves produced by strong-field ionization, Phys. Rev. Lett. 124, 153202 (2020).
- D. Trabert, N. Anders, S. Brennecke, M. S. Schöffler, T. Jahnke, L. P. H. Schmidt, M. Kunitski, M. Lein, R. Dörner, and S. Eckart, Nonadiabatic strong field ionization of atomic hydrogen, Phys. Rev. Lett. 127, 273201 (2021).
- A. Geyer, D. Trabert, M. Hofmann, N. Anders, M. S. Schöffler, L. P. H. Schmidt, T. Jahnke, M. Kunitski, R. Dörner, and S. Eckart, Experimental fingerprint of the electron's longitudinal momentum at the tunnel exit in strong field ionization, Phys. Rev. Res. 5, 033094 (2023).
- M. Hofmann, D. Trabert, A. Geyer, N. Anders, J. Kruse, J. Rist, L. P. H. Schmidt, T. Jahnke, M. Kunitski, M. Schöffler et al., Subcycle resolved strong field ionization of chiral molecules and the origin of chiral photoelectron asymmetries, Phys. Rev. Res. 6, 043176 (2024).
- The values for the electric field shown in Fig. 1 are a.u., a.u., a.u., a.u., , , , , , , , , , , and .
- S. Popruzhenko and D. Bauer, Strong field approximation for systems with Coulomb interaction, J. Mod. Opt. 55, 2573 (2008).
- T.-M. Yan and D. Bauer, Sub-barrier Coulomb effects on the interference pattern in tunneling-ionization photoelectron spectra, Phys. Rev. A 86, 053403 (2012).
- M. V. Ammosov, N. B. Delone, and V. P. Krainov, Tunnel ionization of complex atoms and of atomic ions in an alternating electromagnetic field, Sov. Phys. JETP 64, 1191 (1986).
- H. Zabrodsky and D. Avnir, Continuous symmetry measures. 4. Chirality, J. Am. Chem. Soc. 117, 462 (1995).
- Y. Huismans, A. Rouzée, A. Gijsbertsen, J. H. Jungmann, A. S. Smolkowska, P. S. W. M. Logman, F. Lépine, C. Cauchy, S. Zamith, T. Marchenko, J. M. Bakker, G. Berden, B. Redlich, A. F. G. van der Meer, H. G. Muller, W. Vermin, K. J. Schafer, M. Spanner, M. Y. Ivanov, O. Smirnova et al., Time-resolved holography with photoelectrons, Science 331, 61 (2011).
- D. Rajak, S. Beauvarlet, O. Kneller, A. Comby, R. Cireasa, D. Descamps, B. Fabre, J. D. Gorfinkiel, J. Higuet, S. Petit, S. Rozen, H. Ruf, N. Thiré, V. Blanchet, N. Dudovich, B. Pons, and Y. Mairesse, Laser-induced electron diffraction in chiral molecules, Phys. Rev. X 14, 011015 (2024).
- M. Meckel, A. Staudte, S. Patchkovskii, D. M. Villeneuve, P. B. Corkum, R. Dörner, and M. Spanner, Signatures of the continuum electron phase in molecular strong-field photoelectron holography, Nat. Phys. 10, 594 (2014).
- X. Xie, T. Wang, S. Yu, X. Lai, S. Roither, D. Kartashov, A. Baltuška, X. Liu, A. Staudte, and M. Kitzler, Disentangling intracycle interferences in photoelectron momentum distributions using orthogonal two-color laser fields, Phys. Rev. Lett. 119, 243201 (2017).
- S. Eckart, M. Kunitski, I. Ivanov, M. Richter, K. Fehre, A. Hartung, J. Rist, K. Henrichs, D. Trabert, N. Schlott, L. Ph. H. Schmidt, T. Jahnke, M. S. Schöffler, A. Kheifets, and R. Dörner, Subcycle interference upon tunnel ionization by counter- rotating two-color fields, Phys. Rev. A 97, 041402(R) (2018).
- T. Moitra, L. Konecny, M. Kadek, O. Neufeld, A. Rubio, and M. Repisky, Light-induced persistent electronic chirality in achiral molecules probed with time-resolved electronic circular dichroism spectroscopy, J. Phys. Chem. Lett. 16, 9210 (2025).
- J.-L. Bégin, M. Alsaawy, and R. Bhardwaj, Chiral discrimination by recollision enhanced femtosecond laser mass spectrometry, Sci. Rep. 10, 14074 (2020).
- M. Liu and Y. Liu, Application of the partial-Fourier-transform approach for tunnel ionization of molecules, Phys. Rev. A 93, 043426 (2016).
- A. Ordóñez, P. Vindel-Zandbergen, and D. Ayuso, All-optical coherent control of chiral electronic transitions for highly enantioselective photochemistry, arXiv:2309.02392.
- W. Sun, D. S. Tikhonov, and M. Schnell, Direct observation of time-dependent coherent chiral tunneling dynamics, Phys. Rev. Lett. 134, 123403 (2025).
- A. Geyer, J. Stindl, I. Dwojak, M. Hofmann, N. Anders, P. Roth, P. Daum, J. Kruse, S. M. Jacob, S. Gurevich, N. Wong, M. S. Schöffler, L. P. H. Schmidt, T. Jahnke, R. Dörner, and S. Eckart, “Data for chiral electron momentum distribution upon strong-field ionization of atoms” (Version 1) [Data set], Zenodo (2025), https://doi.org/10.5281/zenodo.15195910.