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Second-harmonic chiroptical scattering spectroscopy from plasmonic nanohelices.

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    Broadband nonlinear optical scattering reveals spectral trends in chiral nanostructures. This study links linear and nonlinear optical activity, enhancing characterization of nanoscale chirality.

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    Area of Science:

    • Nonlinear Optics
    • Plasmonics
    • Nanochemistry

    Background:

    • Chiral harmonic scattering is a nonlinear optical technique for analyzing chiral nanostructures.
    • Current limitations include narrow spectral ranges and limited comparison with linear chiroptical effects.

    Purpose of the Study:

    • To demonstrate broadband second-harmonic (SH) chiroptical scattering for chiral nanostructures.
    • To investigate spectral trends and compare with linear optical properties.
    • To explore the influence of scattering geometry on nonlinear optical signals.

    Main Methods:

    • Utilized gold and silver plasmonic nanohelices.
    • Performed broadband SH chiroptical scattering over a 150 nm fundamental wavelength range (710-860 nm).
    • Resolved nonlinear ellipticity spectra at ten discrete wavelengths and compared different scattering geometries.

    Main Results:

    • Observed distinct spectral trends between gold and silver nanohelices.
    • Found correspondences between linear circular dichroism (CD) spectra and SH ellipticity spectra.
    • Demonstrated geometry-dependent contrast consistent with hyper-Rayleigh scattering.

    Conclusions:

    • Established the feasibility of spectrally-resolved nonlinear chiroptical analysis.
    • Provided insights into the physical links between linear and nonlinear optical activity in plasmonic nanostructures.
    • Validated a minimal model of hyper-Rayleigh scattering for these systems.