- Physical Review Journals
All JournalsPhysics Magazine

Physical Review A

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

Coherent control of chirality flips in HCOOH(A′′)

ChunMei Liu1, Dongming Jia1,*, Yuan Man2,†, and Yonggang Yang3,4

  • *Contact author: dmjia@njupt.edu.cn
  • †Also known as Jörn Manz.
PDF

Phys. Rev. A 114, 033113 – Published 21 September, 2026

DOI: https://doi.org/10.1103/8ndz-tsr9

Abstract

We design laser pulses to transform the oriented model formic acid (HCOOH) from its achiral ground state (A′) to chiral configurations in the first excited state (A′′). Optimal control of the production of the target enantiomer followed by enantiomer flips with highest enantiomeric excess is achieved by means of a linearly polarized laser pulse with optimal duration, field strength, frequency, and direction of polarization. The approach is motivated by effects of directionality of x-ray or laser pulses on different aspects of chirality of HCOOH discovered by the team of Dörner using cold target recoil ion momentum spectroscopy.

View figure in article

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (32)

  1. K. Fehre, S. Eckart, M. Kunitski, M. Pitzer, S. Zeller, C. Janke, D. Trabert, J. Rist, M. Weller, A. Hartung, L. P. H. Schmidt, T. Jahnke, R. Berger, R. Dörner, and M. S. Schöffler, Enantioselective fragmentation of an achiral molecule in a strong laser field, Sci. Adv. 5, eaau7923 (2019).
  2. D. Tsitsonis, F. Trinter, J. B. Williams, K. Fehre, P. V. Demekhin, T. Jahnke, R. Dörner, and M. S. Schöffler, Enantioselective one-photon excitation of formic acid, Phys. Rev. Lett. 133, 093002 (2024).
  3. D. Tsitsonis, M. Kircher, N. M. Novikovskiy, F. Trinter, J. B. Williams, K. Fehre, L. Kaiser, S. Eckart, O. Kreuz, A. Senftleben, P. V. Demekhin, R. Berger, T. Jahnke, M. S. Schöffler, and R. Dörner, Probing instantaneous single-molecule chirality in the planar ground state of formic acid, Phys. Rev. Lett. 136, 043001 (2026).
  4. A. Schild, On the probability density of the nuclei in a vibrationally excited molecule, Front. Chem. 7, 424 (2019).
  5. R. Dörner, V. Mergel, O. Jagutzki, L. Spielberger, J. Ullrich, R. Moshammer, and H. Schmidt-Böcking, Cold target recoil ion momentum spectroscopy: A ‘momentum microscope’ to view atomic collision dynamics, Phys. Rep. 330, 95 (2000).
  6. See Supplemental Material at http://link.aps.org/supplemental/10.1103/8ndz-tsr9 for additional computational details, derivations, and supporting results, which includes Ref. [32].
  7. T. L. Ng and S. Bell, The π*←n transition of formic acid, J. Mol. Spectrosc. 50, 166 (1974).
  8. F. Ioannoni, D. C. Moule, and D. J. Clouthier, Laser spectroscopic and quantum chemical studies of the lowest excited states of formic acid, J. Phys. Chem. 94, 2290 (1990).
  9. P. A. S. Randi, D. F. Pastega, M. H. F. Bettega, N. C. Jones, S. V. Hoffmann, S. Eden, A. S. Barbosa, and P. Limão-Vieira, Electronically excited states of formic acid investigated by theoretical and experimental methods, Spectrochim. Acta, Part A 289, 122237 (2023).
  10. J. R. Rouxel, M. Kowalewski, and S. Mukamel, Photoinduced molecular chirality probed by ultrafast resonant x-ray spectroscopy, Struct. Dyn. 4, 044006 (2017).
  11. D. S. Tikhonov, A. Blech, M. Leibscher, L. Greenman, M. Schnell, and C. P. Koch, Pump-probe spectroscopy of chiral vibrational dynamics, Sci. Adv. 8, eade0311 (2022).
  12. M. Leibscher, E. Pozzoli, A. Blech, M. Sigalotti, U. Boscain, and C. P. Koch, Quantum control of rovibrational dynamics and application to light-induced molecular chirality, Phys. Rev. A 109, 012810 (2024).
  13. J. Wu and H. Zeng, Field-free molecular orientation control by two ultrashort dual-color laser pulses, Phys. Rev. A 81, 053401 (2010).
  14. K. Kitano, N. Ishii, and J. Itatani, High degree of molecular orientation by a combination of THz and femtosecond laser pulses, Phys. Rev. A 84, 053408 (2011).
  15. K. Lin, I. Tutunnikov, J. Qiang, J. Ma, Q. Song, Q. Ji, W. Zhang, H. Li, F. Sun, X. Gong, H. Li, P. Lu, H. Zeng, Y. Prior, I. S. Averbukh, and J. Wu, All-optical field-free three-dimensional orientation of asymmetric-top molecules, Nat. Commun. 9, 5134 (2018).
  16. M. Born and K. Huang, Dynamical Theory of Crystal Lattices (Oxford University Press, Oxford, 1954).
  17. S. Grimme, Semiempirical hybrid density functional with perturbative second-order correlation, J. Chem. Phys. 124, 034108 (2006).
  18. A. D. Becke, Density-functional exchange-energy approximation with correct asymptotic behavior, Phys. Rev. A 38, 3098 (1988).
  19. F. Weigend and R. Ahlrichs, Balanced basis sets of split valence, triple zeta and quadruple zeta valence quality for H to Rn: Design and assessment of accuracy, Phys. Chem. Chem. Phys. 7, 3297 (2005).
  20. M. J. Frisch et al., Gaussian 16, Revision A.03 (Gaussian, Inc., Wallingford, CT, 2016).
  21. C. C. Marston and G. G. Balint-Kurti, The Fourier grid Hamiltonian method for bound state eigenvalues and eigenfunctions, J. Chem. Phys. 91, 3571 (1989).
  22. M. D. Feit, J. A. Fleck, and A. Steiger, Solution of the Schrödinger equation by a spectral method, J. Comput. Phys. 47, 412 (1982).
  23. C. Leforestier, R. H. Bisseling, C. Cerjan, M. D. Feit, R. Friesner, A. Guldberg, A. Hammerich, G. Jolicard, W. Karrlein, H.-D. Meyer, N. Lipkin, O. Roncero, and R. Kosloff, A comparison of different propagation schemes for the time dependent Schrödinger equation, J. Comput. Phys. 94, 59 (1991).
  24. F. Hund, Zur Deutung der Molekelspektren. iii. Bemerkungen über das Schwingungs und Rotationsspektrum bei Molekeln mit mehr als zwei Kernen, Z. Phys. 43, 805 (1927).
  25. S. Kozuch and J. Kästner, Tunnelling in Molecules–Nuclear Quantum Effects from Bio- to Physical Chemistry (The Royal Society of Chemistry, London, 2021).
  26. D. M. Neumark, Transition state spectroscopy in Advanced Series in Physical Chemistry, Modern Trends in Chemical Reaction Dynamics (World Scientific, Singapore, 2004), pp. 453–473.
  27. J. Li, S.-D. Li, J. Manz, H. Wang, and Y. Yang, On the forward-backward symmetry of reversible thermoneutral unimolecular reactions, Chem. Phys. Lett. 871, 142116 (2025).
  28. C. Zhou, T. Kanai, and S. Watanabe, Generation of ultrashort 90µJ deep-ultraviolet pulses by dual broadband frequency doubling with β−BaB2O4 crystals at 1 kHz, Appl. Phys. Express 8, 012701 (2015).
  29. S. W. Grib, P. S. Hsu, H. U. Stauffer, C. D. Carter, and S. Roy, Comparison of femtosecond and nanosecond two-photon-absorption laser-induced fluorescence of krypton, Appl. Opt. 58, 7621 (2019).
  30. X. Xie, S. Soultanis, G. Knopp, A. L. Cavalieri, and S. L. Johnson, Generation of intense ultrashort deep ultraviolet pulses at 200 nm, High Pow. Laser Sci. Eng. 13, e103 (2025).
  31. M. Quack, Spectra and dynamics of coupled vibrations in polyatomic molecules, Annu. Rev. Phys. Chem. 41, 839 (1990).
  32. D. J. Tannor, Introduction to Quantum Mechanics: A Time-Dependent Perspective (University Science Books, Sausalito, CA, 2007), Chaps. 9.2 and 15.1.

Outline

Information

Phys. Rev. A 114, 033113– Published 21 September, 2026
  • Received 26 June 2026
  • Accepted 27 August 2026
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