Journal
LASER & PHOTONICS REVIEWS
Volume 15, Issue 11, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/lpor.202100235
Keywords
chirality; metamaterials; nanophotonics; nonlinear optics; plasmonics
Categories
Funding
- Royal Society
- Royal Society [PEF1\170015, ICA\R1\201088, RGF\EA\180228]
- STFC [ST/R005842/1]
- Engineering and Physical Sciences Research Council (EPSRC) Centre for Doctoral Training in Condensed Matter Physics (CDT-CMP) [EP/L015544/1]
- EPSRC [EP/T001046/1, EPSRC DTP EB-BB1250]
- EPSRC [EP/T001046/1] Funding Source: UKRI
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This study reveals the hidden third-harmonic optical properties upon CPL illumination, referred to as THRS OA, by demonstrating a new effect in hyper-Rayleigh scattering, where the intensity depends on the chirality of the scatterers.
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.
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