Optical activity in third-harmonic Rayleigh scattering: A new route for measuring chirality

Ohnoutek, Lukas, Jeong, Hyeon Ho, Jones, Robin Raffe, Sachs, Johannes, Olohan, Ben J., Răsădean, Dora Maria, Pantoş, Gheorghe Dan, Andrews, David L., Fischer, Peer and Valev, Ventsislav K. (2021) Optical activity in third-harmonic Rayleigh scattering: A new route for measuring chirality. Laser and Photonics Reviews. ISSN 1863-8880

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Abstract

In 3D isotropic liquids, optical third-harmonic generation is forbidden, with circularly polarized light (CPL). Yet the associated nonlinear susceptibility directly influences the optical properties at the fundamental frequency by intensity dependence (Kerr effect). Here, the hidden third-harmonic optical properties upon CPL illumination are revealed by demonstrating a new effect, in hyper-Rayleigh scattering. This effect is succinctly enunciated: the intensity of light scattered at the third-harmonic frequency of the CPL incident light depends on the chirality of the scatterers. It is referred to as third-harmonic (hyper) Rayleigh scattering optical activity (THRS OA) and was observed from Ag nanohelices randomly dispersed in water. The first analytical theory model for the new effect in nanohelices is also provided, highlighting the role of localized transition dipoles along the helical length. THRS OA is remarkably user-friendly. It offers access to intricate optical properties (hyperpolarizabilities) that have so far been more easily accessible by computation and that are essential for the understanding of light−matter interactions. The new effect could find applications in hyper-sensitive characterization of the chirality in molecules and in nanostructures; this chirality plays a fundamental role in the function of bio/nano-machinery, with promising applications in next generation technologies.

Item Type: Article
Additional Information: Funding Information: V.K.V. acknowledges support from the Royal Society through the University Research Fellowships and the Royal Society grants PEF1∖170015, ICA∖R1∖201088, and RGF∖EA∖180228, as well as, the STFC grant ST/R005842/1. 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 No. EP/L015544/1. V.K.V. further acknowledges EPSRC grant EP/T001046/1. D.M.R. and G.D.P. acknowledge support from the EPSRC through grant EPSRC DTP EB‐ BB1250.
Uncontrolled Keywords: chirality,metamaterials,nanophotonics,nonlinear optics,plasmonics,electronic, optical and magnetic materials,atomic and molecular physics, and optics,condensed matter physics ,/dk/atira/pure/subjectarea/asjc/2500/2504
Faculty \ School: Faculty of Science > School of Chemistry
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Depositing User: LivePure Connector
Date Deposited: 30 Sep 2021 19:35
Last Modified: 02 Oct 2021 00:59
URI: https://ueaeprints.uea.ac.uk/id/eprint/81527
DOI: 10.1002/lpor.202100235

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