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Register a new userSpatially resolved enhancement of fluorescence and Raman scattering by Ag nanoparticle arrays
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Highly ordered periodic arrays of silver nanoparticles have been fabricated which exhibit surface plasmon resonances in the visible spectrum. We demonstrate the ability of these structures to alter the fluorescence properties of vicinal dye molecules by providing an additional radiative decay channel. Using fluorescence lifetime imaging microscopy, we have created high resolution spatial maps of the molecular lifetime components; these show an order of magnitude increase in decay rate from a localized volume around the nanoparticles, resulting in a commensurate enhancement in the fluorescence emission intensity. Spatial maps of the Raman scattering signal from molecules on the nanoparticles shows an enhancement of more than 5 orders of magnitude.
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We report modifications to the optical properties of fluorophores in the vicinity of noble metal nanotips. The fluorescence from small clusters of quantum dots has been imaged using an apertureless scanning near-field optical microscope. When a sharp gold tip is brought close to the sample surface, a strong distance-dependent enhancement of the quantum dot fluorescence is observed, leading to a simultaneous increase in optical resolution. These results are consistent with simulations of the electric field and fluorescence enhancement near plasmonic nanostructures. Highly ordered periodic arrays of silver nanotips have been fabricated by nanosphere lithography. Using fluorescence lifetime imaging microscopy, we have created high resolution spatial maps of the lifetime components of vicinal fluorophores; these show an order of magnitude increase in decay rate from a localized volume around the nanotips, resulting in a commensurate enhancement in the fluorescence emission intensity. Spatial maps of the Raman scattering signal from molecules on the nanotips shows an enhancement of more than 5 orders of magnitude.
We have investigated the effects of tuning the localized surface plasmon resonances (LSPRs) of silver nanoparticles on the fluorescence intensity, lifetime, and Raman signal from nearby fluorophores. The presence of a metallic structure can alter the optical properties of a molecule by increasing the excitation field, and by modifying radiative and non-radiative decay mechanisms. By careful choice of experimental parameters we have been able to decouple these effects. We observe a four-fold increase in fluorescence enhancement and an almost 30-fold increase in decay rate from arrays of Ag nanoparticles, when the LSPR is tuned to the emission wavelength of a locally situated fluorophore. This is consistent with a greatly increased efficiency for energy transfer from fluorescence to surface plasmons. Additionally, surface enhanced Raman scattering (SERS) measurements show a maximum enhancement occurs when both the incident laser light and the Raman signal are near resonance with the plasmon energy. Spatial mapping of the SERS signal from a nanoparticle array reveals highly localized differences in the excitation field resulting from small differences in the LSPR energy.
We present a general model study of surface-enhanced resonant Raman scattering and fluorescence focusing on the interplay between electromagnetic effects and the molecular dynamics. Our model molecule is placed close to two Ag nanoparticles, and has two electronic levels. A Franck-Condon mechanism provides electron-vibration coupling. Using realistic parameter values for the molecule we find that an electromagnetic enhancement by 10 orders of magnitude can yield Raman cross-sections $sigma_{R}$ of the order $10^{-14} unit{cm^2}$. We also discuss the dependence of $sigma_{R}$ on incident laser intensity.
Highly ordered periodic arrays of silver nanoparticles have been fabricated which exhibit surface plasmon resonances in the visible spectrum. We demonstrate the ability of these structures to alter the fluorescence properties of vicinal dye molecules by providing an additional radiative decay channel. Using fluorescence lifetime imaging microscopy (FLIM), we have created high resolution spatial maps of the molecular lifetime components; these show an order of magnitude increase in decay rate from a localized volume around the nanoparticles, resulting in a commensurate enhancement in the fluorescence emission intensity.
We present angle and frequency resolved optical extinction measurements to determine the dispersion relation of plasmon modes on Ag and Au nanoparticle chains with pitches down to 75 nm. The large splitting between transverse and longitudinal modes and the band curvature are inconsistent with reported electrostatic near-field models, and confirm that far-field retarded interactions are important, even for $lambda/5$-sized structures. The data imply that lower propagation losses, larger signal bandwidth and larger maximum group velocity then expected can be achieved for wave vectors below the light line. We conclude that for the design of optical nanocircuits coherent far-field couplings across the entire circuit need to be considered, even at subwavelength feature sizes.
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