- Open Access
Bottom-up Analysis of Rovibrational Helical Dichroism
Phys. Rev. Lett. 136, 053204 – Published 5 February, 2026
DOI: https://doi.org/10.1103/fkf1-1jml
Abstract
We present a general theoretical framework for helical dichroism (HD), establishing an explicit link between chiral resolution and orbital angular momentum (OAM) exchange in light–matter interaction. Tracing microscopic mechanisms of the OAM transfer, we derive rotational selection rules, which establish that HD emerges only from the spin–orbit coupling of light, even for beams without the far-field OAM. Our findings refine the conditions for observing HD, provide a tool to re-examine the outcome of prior experiments, and guide future designs for chiral sensing with structured light.
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References (46)
- N. M. Maier, P. Franco, and W. Lindner, Separation of enantiomers: Needs, challenges, perspectives, J. Chromatogr. A 906, 3 (2001).
- H. M. Barkholtz, R. Hadzima, and A. Miles, Pharmacology of R-(-)-methamphetamine in humans: A systematic review of the literature, ACS Pharmacol. Transl. Sci. 6, 914 (2023).
- J. M. Brown and S. G. Davies, Chemical asymmetric synthesis, Nature (London) 342, 631 (1989).
- H.-L. Qian, S.-T. Xu, and X.-P. Yan, Recent advances in separation and analysis of chiral compounds, Anal. Chem. 95, 304 (2023).
- C. P. Koch, M. Lemeshko, and D. Sugny, Quantum control of molecular rotation, Rev. Mod. Phys. 91, 035005 (2019).
- C. W. Deutsche and A. Moscowitz, Optical activity of vibrational origin. II. Consequences of polymer conformation, J. Chem. Phys. 53, 2630 (1970).
- G. Holzwarth, E. C. Hsu, H. S. Mosher, T. R. Faulkner, and A. Moscowitz, Infrared circular dichroism of carbon-hydrogen and carbon-deuterium stretching modes. Observations, J. Am. Chem. Soc. 96, 251 (1974).
- A. J. Miles, R. W. Janes, and B. A. Wallace, Tools and methods for circular dichroism spectroscopy of proteins: A tutorial review, Chem. Soc. Rev. 50, 8400 (2021).
- L. Allen, M. W. Beijersbergen, R. J. C. Spreeuw, and J. P. Woerdman, Orbital angular momentum of light and the transformation of Laguerre-Gaussian laser modes, Phys. Rev. A 45, 8185 (1992).
- K. A. Forbes and D. L. Andrews, Orbital angular momentum of twisted light: Chirality and optical activity, J. Phys. Photonics 3, 022007 (2021).
- D. Andrews, L. Romero, and M. Babiker, On optical vortex interactions with chiral matter, Opt. Commun. 237, 133 (2004).
- L. Ye, J. R. Rouxel, S. Asban, B. Rösner, and S. Mukamel, Probing molecular chirality by orbital-angular-momentum-carrying x-ray pulses, J. Chem. Theory Comput. 15, 4180 (2019).
- M. Li, S. Yan, Y. Zhang, X. Chen, and B. Yao, Optical separation and discrimination of chiral particles by vector beams with orbital angular momentum, Nanoscale Adv. 3, 6897 (2021).
- K. A. Forbes and D. L. Andrews, Optical orbital angular momentum: twisted light and chirality, Opt. Lett. 43, 435 (2018).
- K. A. Forbes and D. L. Andrews, Spin-orbit interactions and chiroptical effects engaging orbital angular momentum of twisted light in chiral and achiral media, Phys. Rev. A 99, 023837 (2019).
- K. A. Forbes, On the transfer of optical orbital angular momentum to matter, arXiv:2101.10660.
- F. Araoka, T. Verbiest, K. Clays, and A. Persoons, Interactions of twisted light with chiral molecules: An experimental investigation, Phys. Rev. A 71, 055401 (2005).
- W. Löffler, D. J. Broer, and J. P. Woerdman, Circular dichroism of cholesteric polymers and the orbital angular momentum of light, Phys. Rev. A 83, 065801 (2011).
- E. Rusak, J. Straubel, P. Gładysz, M. Göddel, A. Kedziorski, M. Kühn, F. Weigend, C. Rockstuhl, and K. Słowik, Enhancement of and interference among higher order multipole transitions in molecules near a plasmonic nanoantenna, Nat. Commun. 10, 5775 (2019).
- X. Zhang and T. J. Cui, Single-particle dichroism using orbital angular momentum in a microwave plasmonic resonator, ACS Photonics 7, 3291 (2020).
- J. R. Rouxel, B. Rösner, D. Karpov, C. Bacellar, G. F. Mancini, F. Zinna, D. Kinschel, O. Cannelli, M. Oppermann, C. Svetina, A. Diaz, J. Lacour, C. David, and M. Chergui, Hard X-ray helical dichroism of disordered molecular media, Nat. Photonics 16, 570 (2022).
- J.-L. Bégin, A. Jain, A. Parks, F. Hufnagel, P. Corkum, E. Karimi, T. Brabec, and R. Bhardwaj, Nonlinear helical dichroism in chiral and achiral molecules, Nat. Photonics 17, 82 (2023).
- A. Jain, J.-L. Bégin, and R. Bhardwaj, Helical dichroism in enantiomeric solutions, J. Chem. Phys. 159, 014504 (2023).
- M. Maslov, G. M. Koutentakis, M. Hrast, O. H. Heckl, and M. Lemeshko, Theory of angular momentum transfer from light to molecules, Phys. Rev. Res. 6, 033277 (2024).
- M. Maslov, Emergent physics of rotating quantum impurities in many-body environments, Ph.D. thesis, Institute of Science and Technology Austria (ISTA), 2025, 10.15479/at:ista:19048.
- K. Y. Bliokh, F. J. Rodríguez-Fortuño, F. Nori, and A. V. Zayats, Spin–orbit interactions of light, Nat. Photonics 9, 796 (2015).
- P. J. Stephens, Theory of vibrational circular dichroism, J. Phys. Chem. 89, 748 (1985).
- A. Buckingham, P. Fowler, and P. Galwas, Velocity-dependent property surfaces and the theory of vibrational circular dichroism, Chem. Phys. 112, 1 (1987).
- J. Mun and J. Rho, Importance of higher-order multipole transitions on chiral nearfield interactions, Nanophotonics 8, 941 (2019).
- S. W. Lovesey, J. T. Collins, and S. P. Collins, Superchiral photons unveil magnetic circular dichroism, Phys. Rev. B 99, 054428 (2019).
- D. Patterson and J. M. Doyle, Sensitive chiral analysis via microwave three-wave mixing, Phys. Rev. Lett. 111, 023008 (2013).
- D. Patterson, M. Schnell, and J. M. Doyle, Enantiomer-specific detection of chiral molecules via microwave spectroscopy, Nature (London) 497, 475 (2013).
- A. F. Ordonez and O. Smirnova, Generalized perspective on chiral measurements without magnetic interactions, Phys. Rev. A 98, 063428 (2018).
- D. Ayuso, A. F. Ordonez, P. Decleva, M. Ivanov, and O. Smirnova, Strong chiral response in non-collinear high harmonic generation driven by purely electric-dipole interactions, Opt. Express 30, 4659 (2022).
- C.-Y. Ji, S. Xu, Q. Liang, X. Zhang, X. Hong, Y. Wang, X. Li, L. Jiang, Y. Wang, J. Ni, D. Wu, and J. Li, Observation of magnetic quadrupole endowed helical dichroism in artificial propeller meta-molecules, Adv. Opt. Mater. 12, 2302795 (2024).
- See Supplemental Material at http://link.aps.org/supplemental/10.1103/fkf1-1jml, which contains Refs. [24–26,37,38].
- K. Y. Bliokh et al., Roadmap on structured waves, J. Opt. 25, 103001 (2023).
- M. Lax, W. H. Louisell, and W. B. McKnight, From Maxwell to paraxial wave optics, Phys. Rev. A 11, 1365 (1975).
- P. F. Bernath, Spectra of Atoms and Molecules (Oxford University Press, New York, 2005).
- K. A. Forbes and G. A. Jones, Optical vortex dichroism in chiral particles, Phys. Rev. A 103, 053515 (2021).
- K. A. Forbes, D. Green, and G. A. Jones, Relevance of longitudinal fields of paraxial optical vortices, J. Opt. 23, 075401 (2021).
- A. D. Buckingham and M. B. Dunn, Optical activity of oriented molecules, J. Chem. Soc. A, 1988 (1971).
- E. A. Power, Two-photon circular dichroism, J. Chem. Phys. 63, 1348 (1975).
- J.-L. Bégin, E. Karimi, P. Corkum, T. Brabec, and R. Bhardwaj, Orbital angular momentum control of strong-field ionization in atoms and molecules, Nat. Commun. 16, 2467 (2025).
- M. Leibscher, E. Pozzoli, C. Pérez, M. Schnell, M. Sigalotti, U. Boscain, and C. Koch, Full quantum control of enantiomer-selective state transfer in chiral molecules despite degeneracy, Commun. Phys. 5, 110 (2022).
- M. Hrast, G. M. Koutentakis, M. Maslov, and M. Lemeshko, The data that support the findings of this article are openly available at https://zenodo.org/records/17864838 (2025).