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

Optical chirality in Raman scattering

Yi-Jing Wu1, Jing-Han Zhuang1, Zi-Qiang Wang1, Yin-Mei Li1, and Lei Gong1,2,3,*

  • *Contact author: leigong@ustc.edu.cn

Phys. Rev. Research 7, 043011 – Published 2 October, 2025

DOI: https://doi.org/10.1103/b7bv-fpz9

Abstract

Raman optical activity (ROA) offers a powerful tool for distinguishing chiral molecules. However, the inherent properties of light that unveil the “handedness” of molecules remain unclear in the realm of ROA. Here, we find two optical measures—the optical chirality tensor and the optical quadrupole tensor—that contribute to ROA excitations. Subsequently, we propose a theoretical framework to elucidate the relationship between the optical chirality quantities and their molecular counterparts in Raman scattering. This framework allows for more selective and tunable ROA excitations. As a demonstration, we identify linearly polarized standing waves as a good configuration for superchiral ROA excitations, where the optical chirality is locally enhanced. Our work provides insights into optical chirality and paves the way to precisely manipulate chiroptical responses.

View figure in article

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (40)

  1. Y. R. Liu, Z. L. Wu, D. W. Armstrong, H. Wolosker, and Y. B. Zheng, Detection and analysis of chiral molecules as disease biomarkers, Nat. Rev. Chem. 7, 355 (2023).
  2. K. Harrison, A. S. Mackay, L. Kambanis, J. W. C. Maxwell, and R. J. Payne, Synthesis and applications of mirror-image proteins, Nat. Rev. Chem. 7, 383 (2023).
  3. N. Liu and T. Liedl, DNA-assembled advanced plasmonic architectures, Chem. Rev. 118, 3032 (2018).
  4. M. Hentschel, M. Schäferling, X. Y. Duan, H. Giessen, and N. Liu, Chiral plasmonics, Sci. Adv. 3, e1602735 (2017).
  5. D. Patterson, M. Schnell, and J. M. Doyle, Enantiomer-specific detection of chiral molecules via microwave spectroscopy, Nature (London) 497, 475 (2013).
  6. L. D. Barron, Parity and optical activity, Nature (London) 238, 17 (1972).
  7. M. F. Maestre, C. Bustamante, T. L. Hayes, J. A. Subirana, and I. Tinoco, Differential scattering of circularly polarized light by the helical sperm head from the octopus Eledone cirrhosa, Nature (London) 298, 773 (1982).
  8. M. K. Hargreaves, Optical rotatory dispersion—its nature and origin, Nature (London) 195, 560 (1962).
  9. T. M. Lowry, The origin of optical rotatory power, Nature (London) 136, 191 (1935).
  10. W. B. Gratzer and D. A. Cowburn, Optical activity of biopolymers, Nature (London) 222, 426 (1969).
  11. I. Warnke and F. Furche, Circular dichroism: Electronic, Wiley Interdiscip. Rev. Comput. Mol. Sci. 2, 150 (2012).
  12. L. D. Barron and A. D. Buckingham, Rayleigh and Raman scattering from optically active molecules, Mol. Phys. 20, 1111 (1971).
  13. L. D. Barron, M. P. Bogaard, and A. D. Buckingham, Differential Raman scattering of right and left circularly polarized light by asymmetric molecules, Nature (London) 241, 113 (1973).
  14. E. W. Blanch, L. Hecht, and L. D. Barron, Vibrational Raman optical activity of proteins, nucleic acids, and viruses, Methods 29, 196 (2003).
  15. S. Y. Zhu and M. T. Sun, Electronic circular dichroism and Raman optical activity: Principle and applications, Appl. Spectrosc. Rev. 56, 553 (2021).
  16. J. Haesler, I. Schindelholz, E. Riguet, C. G. Bochet, and W. Hug, Absolute configuration of chirally deuterated neopentane, Nature (London) 446, 526 (2007).
  17. L. H. McColl, E. W. Blanch, A. C. Gill, A. G. O. Rhie, M. A. Ritchie, L. Hecht, K. Nielsen, and L. D. Barron, A new perspective on β-sheet structures using vibrational Raman optical activity: From poly(L-lysine) to the prion protein, J. Am. Chem. Soc. 125, 10019 (2003).
  18. J. Mun, M. Kim, Y. Yang, T. Badloe, J. C. Ni, Y. Chen, C. W. Qiu, and J. Rho, Electromagnetic chirality: From fundamentals to nontraditional chiroptical phenomena, Light Sci. Appl. 9, 139 (2020).
  19. 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).
  20. S. Bordács et al., Chirality of matter shows up via spin excitations, Nat. Phys. 8, 734 (2012).
  21. J. C. Ni et al., Gigantic vortical differential scattering as a monochromatic probe for multiscale chiral structures, Proc. Nat. Acad. Sci. USA 118, e2020055118 (2021).
  22. 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. Photon. 17, 82 (2023).
  23. Y. Q. Tang and A. E. Cohen, Optical chirality and its interaction with matter, Phys. Rev. Lett. 104, 163901 (2010).
  24. N. Yang and A. E. Cohen, Local geometry of electromagnetic fields and its role in molecular multipole transitions, J. Phys. Chem. B 115, 5304 (2011).
  25. Y. Q. Tang and A. E. Cohen, Enhanced enantioselectivity in excitation of chiral molecules by superchiral light, Science 332, 333 (2011).
  26. L. D. Barron, Molecular Light Scattering and Optical Activity (Cambridge University Press, New York, 2009).
  27. L. D. Barron, L. Hecht, I. H. McColl, and E. W. Blanch, Raman optical activity comes of age, Mol. Phys. 102, 731 (2004).
  28. L. Hecht and L. A. Nafie, Theory of natural Raman optical activity. 1. Complete circular polarization formalism, Mol. Phys. 72, 441 (1991).
  29. R. P. Cameron, S. M. Barnett, and A. M. Yao, Optical helicity, optical spin and related quantities in electromagnetic theory, New J. Phys. 14, 053050 (2012).
  30. D. M. Lipkin, Existence of a new conservation law in electromagnetic theory, J. Math. Phys. 5, 696 (1964).
  31. See Supplemental Material at http://link.aps.org/supplemental/10.1103/b7bv-fpz9 for derivations of Eqs.  (6) and (7) and the related discussion of optical chirality.
  32. A. D. Buckingham and M. B. Dunn, Optical activity of oriented molecules, J. Chem. Soc. A 1988 (1971).
  33. A. D. Buckingham and R. E. Raab, Electric-field-induced differential scattering of right and left circularly polarized light, Proc. R. Soc. Lond. A 345, 365 (1975).
  34. K. A. Forbes and D. L. Andrews, Orbital angular momentum of twisted light: Chirality and optical activity, J. Phys. Photon. 3, 022007 (2021).
  35. L. D. Barron and A. D. Buckingham, Rayleigh and Raman optical activity, Annu. Rev. Phys. Chem. 26, 381 (1975).
  36. K. A. Forbes, Raman optical activity using twisted photons, Phys. Rev. Lett. 122, 103201 (2019).
  37. D. Habibovic, K. R. Hamilton, O. Neufeld, and L. Rego, Emerging tailored light sources for studying chirality and symmetry, Nat. Rev. Phys. 6, 663 (2024).
  38. H. F. Hu, Q. Q. Gan, and Q. W. Zhan, Generation of a nondiffracting superchiral optical needle for circular dichroism imaging of sparse subdiffraction objects, Phys. Rev. Lett. 122, 223901 (2019).
  39. C. L. He, G. Yang, Y. Kuai, S. Z. Shan, L. Yang, J. G. Hu, D. G. Zhang, Q. J. Zhang, and G. Zou, Dissymmetry enhancement in enantioselective synthesis of helical polydiacetylene by application of superchiral light, Nat. Commun. 9, 5117 (2018).
  40. A. Biswas, P. Cencillo-Abad, M. W. Shabbir, M. Karmakar, and D. Chanda, Tunable plasmonic superchiral light for ultrasensitive detection of chiral molecules, Sci. Adv. 10, eadk2560 (2024).

Outline

Information

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation