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Nonlinear helical dichroism in chiral and achiral molecules

Nature Photonics volume 17, pages 82–88 (2023)Cite this article

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Abstract

Chiral interactions are prevalent in nature, driving a variety of biochemical processes. Discerning the two non-superimposable mirror images of a chiral molecule, known as enantiomers, requires interaction with a chiral reagent with known handedness. Circularly polarized light beams are often used as a chiral reagent. Here we demonstrate efficient chiral sensitivity with linearly polarized helical light beams carrying an orbital angular momentum of ±lħ, in which the handedness is defined by the twisted wavefront structure tracing a left- or right-handed corkscrew pattern as it propagates in space. By probing the nonlinear optical response, we show that helicity-dependent nonlinear absorption occurs even in achiral molecules and can be controlled. We model this effect by considering induced multipole moments in light–matter interactions. Design and control of light–matter interactions with helical light may open new opportunities in chiroptical spectroscopy, light-driven molecular machines, optical switching and in situ ultrafast probing of chiral systems and magnetic materials.

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Fig. 1: Transmission of circularly polarized (s = ±1) femtosecond vortex pulses in fenchone.
Fig. 2: Helical dichroism (Type II) in fenchone with linearly polarized light (s = 0) as a function of peak laser fluence.
Fig. 3: Helicity-dependent absorption, HD(Type I), in achiral molecules.
Fig. 4: Helical dichroism with linearly polarized asymmetric OAM beams (l = ±1) in limonene.
Fig. 5: Helical dichroism (Type I) with asymmetric OAM beams in R(+)-limonene.

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The minimum dataset necessary to interpret the results can be obtained from the corresponding authors upon reasonable request.

Code availability

The simulation data were obtained by evaluating the equations using standard technical software. The code is available upon reasonable request to the corresponding authors.

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Acknowledgements

We acknowledge financial support from the Natural Science and Engineering Council of Canada, Canada Research Chairs and Canadian Foundation for Innovation.

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  1. These authors contributed equally: Jean-Luc Bégin, Ashish Jain.

Authors and Affiliations

  1. Department of Physics, University of Ottawa, Ottawa, Ontario, Canada

    Jean-Luc Bégin, Ashish Jain, Andrew Parks, Felix Hufnagel, Paul Corkum, Ebrahim Karimi, Thomas Brabec & Ravi Bhardwaj

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Contributions

J-L.B., A.J. and R.B. conceived the experiments. J-L.B., A.J. and R.B. designed and planned the experiments. J-L.B. and A.J. conducted the experiments and analysed the results. J-L.B., A.J., A.P., T.B. and R.B. worked on the theory and conducted numerical simulations. F.H. fabricated the q-plates, P.C., E.K. and R.B. supervised the project. J-L.B., A.J., T.B. and R.B. prepared the first draft, and all authors reviewed the manuscript.

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Correspondence to Ravi Bhardwaj.

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Nature Photonics thanks David Andrews and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Information

Supplementary Information, including ten sections. Additional results are provided in sections 1 to 7, including Figs. 1–8. The Discussion includes three sections: fluence calculations with Fig. 9, optical force dipole with Fig. 10 and the theory on extension to multiphotons.

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Bégin, JL., Jain, A., Parks, A. et al. Nonlinear helical dichroism in chiral and achiral molecules. Nat. Photon. 17, 82–88 (2023). https://doi.org/10.1038/s41566-022-01100-0

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