Synthetic chiral light for efficient control of chiral light–matter interaction

Abstract

Light is a very powerful and precise tool, allowing us to control1, shape2,3 and create new phases4 of matter. In such tasks, the magnetic component of a light wave is essential in defining the wave’s helicity, but it influences the optical response of matter only weakly. Chiral molecules offer a typical example, in which the weakness of magnetic interactions hampers our ability to control the strength of their chiro-optical response5, limiting it at several orders of magnitude below the full potential. Here, we introduce and theoretically analyse a new type of chiral light: freely propagating, locally and globally chiral electric fields, which interact with chiral matter extremely efficiently. We show that this synthetic chiral light enables full control over the intensity, polarization and propagation direction of the nonlinear enantio-sensitive optical response of randomly oriented chiral molecules. This response can be quenched or enhanced at will in a desired enantiomer, opening up efficient ways to control chiral matter and for ultrafast imaging of chiral dynamics in gases, liquids and solids.

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Fig. 1: Synthetic chiral light.
Fig. 2: Practical set-up.
Fig. 3: Chiral response in HHG using standard chiral light.
Fig. 4: Near-field enantio-sensitive HHG using synthetic chiral light.
Fig. 5: Far-field harmonic intensity and chiral dichroism.

Data availability

The data that support the plots within this paper and other findings of this study are available from the corresponding authors upon reasonable request.

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Acknowledgements

We thank F. Morales for discussions. D.A., A.F.O. and O.S. acknowledge support from the DFG SPP 1840 ‘Quantum Dynamics in Tailored Intense Fields’ and DFG grant SM 292/5-2; A.F.O. and O.S. acknowledge support from MEDEA. The MEDEA project has received funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement no. 641789. This work was supported by the Israel Science Foundation (grant no. 1781/18) and the Wolfson Foundation. O.N. acknowledges the support of the Adams Fellowship Program of the Israel Academy of Sciences and Humanities.

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D.A., A.F.O. and O.S. developed the concepts of locally and globally chiral fields. D.A., A.F.O. and O.S. developed the theory of chiral correlation functions. O.N., G.L. and O.C. developed a concept of reflection and inversion free fields, which are locally chiral, and the group theory-based analysis of such fields. O.N. proved the connection between the symmetry-based description of locally chiral fields and reflection and inversion free fields. O.N. and O.C. formulated the degree of chirality of light fields. D.A., P.D., M.I. and O.S. developed and computed the hybrid DFT–strong-field description of the microscopic and macroscopic HHG response in propylene oxide. O.N. computed the DFT-based microscopic HHG response in bromochlorofluoromethane. D.A., A.F.O., M.I. and O.S. wrote the initial version of the manuscript. All authors contributed to writing the manuscript.

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Correspondence to David Ayuso or Misha Ivanov or Olga Smirnova.

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Ayuso, D., Neufeld, O., Ordonez, A.F. et al. Synthetic chiral light for efficient control of chiral light–matter interaction. Nat. Photonics 13, 866–871 (2019). https://doi.org/10.1038/s41566-019-0531-2

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