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Third-harmonic Mie scattering from semiconductor nanohelices

Nature Photonics volume 16, pages 126–133 (2022)Cite this article

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Abstract

Chiroptical spectroscopies provide structural analyses of molecules and nanoparticles but they require sample volumes that are incompatible with generating large chemical libraries. New optical tools are needed to characterize chirality for the ultrasmall (<1 µl) volumes required in the high-throughput synthetic and analytical stations for chiral compounds. Here we show experimentally a novel photonic effect that enables such capabilities—third-harmonic Mie scattering optical activity—observed from suspensions of CdTe nanostructured helices in volumes <<1 µl. Third-harmonic Mie scattering was recorded on illuminating CdTe helices with 1,065, 1,095 and 1,125 nm laser beams and the intensity was around ten-times higher in the forward direction than sideways. The third-harmonic ellipticity was as high as 3° and we attribute this effect to the interference of chiral and achiral effective nonlinear susceptibility tensor components. Third-harmonic Mie scattering on semiconductor helices opens a path for rapid high-throughput chiroptical characterization of sample volumes as small as 10−5 µl.

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Fig. 1: CdTe nanohelices for third-harmonic Mie scattering optical activity.
Fig. 2: Demonstration of THMS optical activity.
Fig. 3: Confirmation of THMS optical activity.
Fig. 4: Applications of THMS for characterizing chiral nanostructures in ultrasmall volumes.

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Data availability

All data supporting this study are openly available from the University of Bath Research Data Archive at https://doi.org/10.15125/BATH-01005 (ref. 58).

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Acknowledgements

We are grateful to D. Carbery for providing cuvettes with 1 mm pathlength. V.K.V. acknowledges support from the Royal Society through the University Research Fellowships, the Royal Society grants PEF1\170015, RF\ERE\210172, ICA\R1\201088 and RGF\EA\180228, the STFC grant ST/R005842/1 and the EPSRC grant EP/T001046/1. L.O. and V.K.V. acknowledge funding and support from the Engineering and Physical Sciences Research Council (EPSRC) Centre for Doctoral Training in Condensed Matter Physics (CDT-CMP), grant EP/L015544/1. N.A.K acknowledges the Vannevar Bush DoD Fellowship to N.A.K. titled Engineered Chiral Ceramics, ONR N000141812876, and ONR COVID-19 Newton Award Pathways to Complexity with Imperfect Nanoparticles, HQ00342010033. D.M.R. and G.D.P. acknowledge support from the EPSRC through grant EPSRC DTP EB- BB1250.

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Author notes

  1. These authors contributed equally: Lukas Ohnoutek, Ji-Young Kim.

Authors and Affiliations

  1. Centre for Photonics and Photonic Materials, University of Bath, Bath, UK

    Lukas Ohnoutek, Ben J. Olohan & Ventsislav K. Valev

  2. Centre for Nanoscience and Nanotechnology, University of Bath, Bath, UK

    Lukas Ohnoutek, Ben J. Olohan & Ventsislav K. Valev

  3. Department of Chemical Engineering, University of Michigan, Ann Arbor, MI, USA

    Ji-Young Kim, Jun Lu & Nicholas A. Kotov

  4. Biointerfaces Institute, University of Michigan, Ann Arbor, MI, USA

    Ji-Young Kim, Jun Lu & Nicholas A. Kotov

  5. Department of Chemistry, University of Bath, Bath, UK

    Dora M. Răsădean & G. Dan Pantoș

  6. Centre for Therapeutic Innovation, University of Bath, Bath, UK

    Ventsislav K. Valev

  7. Department of Basic and Applied Sciences for Engineering, the Sapienza University of Rome, Rome, Italy

    Ventsislav K. Valev

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  1. Lukas Ohnoutek
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Contributions

V.K.V. and N.A.K. conceived the experiments. L.O., V.K.V. and B.O. performed the nonlinear optical experiments. J-Y.K., J.L. and N.A.K. prepared and provided the samples. L.O., D.M.R. and G.D.P. performed the linear optical experiments. J-Y.K. performed the numerical simulations. L.O., J-Y.K., N.A.K. and V.K.V. analysed the data. L.O. and V.K.V. wrote the first draft and all authors contributed towards writing the paper.

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Correspondence to Nicholas A. Kotov or Ventsislav K. Valev.

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Ohnoutek, L., Kim, JY., Lu, J. et al. Third-harmonic Mie scattering from semiconductor nanohelices. Nat. Photon. 16, 126–133 (2022). https://doi.org/10.1038/s41566-021-00916-6

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