期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 126, 期 24, 页码 10129-10138出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.2c02128
关键词
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资金
- Rutherford Discovery Fellowship
- Marsden Grant of the Royal Society New Zealand
The research investigates the impact of adsorbed molecule orientation and position on the surface of metallic nanoparticles on the sensitivity of localized surface plasmon resonance (LSPR) sensing. Results show that molecules with their main optical axis perpendicular to the surface and located near hot spots can induce a significantly larger resonance shift, suggesting potential improvements in LSPR sensing sensitivity through targeted adsorption at hot spots with carefully engineered molecular orientation.
Localized surface plasmon resonances (LSPRs) of metallic nanoparticles are affected by their surroundings and in particular by the presence of adsorbed molecules on their surface. This effect is central to their application in LSPR sensing. We here investigate how the adsorbed molecule orientation on the surface and position, notably with respect to an electromagnetic hot spot, affect the amplitude of the resonance shift, and therefore the LSPR sensing sensitivity. We use a recently developed effective anisotropic dielectric function describing a homogeneous shell of adsorbed molecules combined with anisotropic Mie theory calculations for core-shell spherical systems or finite-element modeling for nonspherical or partial shell configurations. We show that the induced plasmon resonance shift per molecule is strongly correlated with the near-field enhancement experienced by the adsorbed molecules. Molecules with their main optical axis perpendicular to the surface and those located at hot spots can therefore induce a much larger resonance shift, by at least 1 order of magnitude. This work suggests that large improvements in LSPR sensing sensitivity could be achieved with new schemes including targeted adsorption at hot spots with carefully engineered molecular orientation.
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