Abstract
In biology, sensing is a major driver of discovery. A principal challenge is to create a palette of probes that offer near single-molecule sensitivity and simultaneously enable multiplexed sensing and imaging in the “tissue-transparent” near-infrared region. Surface-enhanced Raman scattering and metal-enhanced fluorescence have shown substantial promise in addressing this need. Here, we theorize a rational design and optimization strategy to generate nanostructured probes that combine distinct plasmonic materials sandwiching a dielectric layer in a multilayer core shell configuration. The lower energy resonance peak in this multi-resonant construct is found to be highly tunable from visible to the near-IR region. Such a configuration also allows substantially higher near-field enhancement, compared to a classical core-shell nanoparticle that possesses a single metallic shell, by exploiting the differential coupling between the two core-shell interfaces. Combining such structures in a dimer configuration, which remains largely unexplored at this time, offers significant opportunities not only for near-field enhancement but also for multiplexed sensing via the (otherwise unavailable) higher order resonance modes. Together, these theoretical calculations open the door for employing such hybrid multi-layered structures, which combine facile spectral tunability with ultrahigh sensitivity, for biomolecular sensing.
Highlights
In biology, sensing is a major driver of discovery
Structure composed of a 40 nm silver nanosphere covered by a dielectric shell and a gold shell, each having a thickness of 10 nm
Our selection of the core and two shell materials were governed by the higher EM enhancement capabilities of silver and the superior biocompatibility of gold, respectively.The choice of dielectric material will depend on the specific application, and the reporter molecule to be functionalized
Summary
In biology, sensing is a major driver of discovery. A principal challenge is to create a palette of probes that offer near single-molecule sensitivity and simultaneously enable multiplexed sensing and imaging in the “tissue-transparent” near-infrared region. The lower energy resonance peak in this multi-resonant construct is found to be highly tunable from visible to the near-IR region Such a configuration allows substantially higher near-field enhancement, compared to a classical core-shell nanoparticle that possesses a single metallic shell, by exploiting the differential coupling between the two core-shell interfaces. Combining such structures in a dimer configuration, which remains largely unexplored at this time, offers significant opportunities for near-field enhancement and for multiplexed sensing via the (otherwise unavailable) higher order resonance modes. Using MCS structures, similar optical characteristics as a CS structure can be achieved in smaller sizes that would allow better targeting ability and pharmacokinetics in vivo, as larger probes often face significant hindrances in reaching their targeted location[26]
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