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Modal interference in spiky nanoshells.

Simon P Hastings, Zhaoxia Qian, Pattanawit Swanglap

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    Summary
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    We developed a new method using T-matrix calculations to understand how plasmonic modes couple in metallic nanostructures. This helps explain strong electric field enhancements for applications like Quadrupole Enhanced Raman Scattering (QERS).

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    Area of Science:

    • Plasmonics and Nanophotonics
    • Computational Electromagnetics

    Background:

    • Metallic nanostructures enable near-field electric field enhancement crucial for non-linear optics, like surface-enhanced Raman scattering.
    • Coupling dark plasmonic modes with dipolar resonators is key for strong electric field localization, but challenging to predict in complex nanostructures.

    Purpose of the Study:

    • To develop a robust method for calculating the T-matrix, which predicts scattered electric fields.
    • To quantify the coupling between electric dipole and quadrupole modes in spiky nanoshells.
    • To understand the origin of spectrally broad quadrupole resonances leading to Quadrupole Enhanced Raman Scattering (QERS).

    Main Methods:

    • Utilized finite-difference time-domain (FDTD) simulations.
    • Employed least-square fitting algorithms to solve the T-matrix.
    • Calculated the T-matrix across a broad spectral range.
    • Performed single-particle backscattering measurements.

    Main Results:

    • Developed a robust T-matrix calculation method applicable over broad spectra.
    • Evaluated coupling between dipole and quadrupole modes in spiky nanoshells.
    • Disorder in spiky nanoshells facilitates coupling between dipole modes and between dipole and quadrupole modes.
    • A ~5% coupling strength explains observed interference features in scattering spectra.

    Conclusions:

    • The T-matrix method provides a robust way to characterize plasmonic mode coupling.
    • Modal interference in disordered spiky nanoshells explains broad quadrupole resonances.
    • This understanding is vital for optimizing nanostructures for enhanced Quadrupole Enhanced Raman Scattering (QERS).