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Register a new userUnified treatment of fluorescence and Raman scattering processes near metal surfaces
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Hongxing Xu
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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.
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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.
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.
We introduce a simple two region model where the diffusion constant in a small region around each step on a vicinal surface can differ from that found on the terraces. Steady state results for this model provide a physically suggestive mapping onto kinetic coefficients in the conventional sharp-step model, with a negative coefficient arising from faster diffusion in the step region. A linear stability analysis of the resulting sharp-step model provides a unified and simple interpretation of many experimental results for current-induced step bunching and wandering instabilities on both Si(111) and Si(001) surfaces.
In metal-enhanced fluorescence (MEF), the localized surface plasmon resonances of metallic nanostructures amplify the absorption of excitation light and assist in radiating the consequent fluorescence of nearby molecules to the far-field. This effect is at the base of various technologies that have strong impact on fields such as optics, medical diagnostics and biotechnology. Among possible emission bands, those in the near-infrared (NIR) are particularly intriguing and widely used in proteomics and genomics due to its noninvasive character for biomolecules, living cells, and tissues, which greatly motivates the development of effective, and eventually multifunctional NIR-MEF platforms. Here we demonstrate NIR-MEF substrates based on Au nanocages micropatterned with a tight spatial control. The dependence of the fluorescence enhancement on the distance between the nanocage and the radiating dipoles is investigated experimentally and modeled by taking into account the local electric field enhancement and the modified radiation and absorption rates of the emitting molecules. At a distance around 80 nm, a maximum enhancement up to 2-7 times with respect to the emission from pristine dyes (in the region 660 nm-740 nm) is estimated for films and electrospun nanofibers. Due to their chemical stability, finely tunable plasmon resonances, and large light absorption cross sections, Au nanocages are ideal NIR-MEF agents. When these properties are integrated with the hollow interior and controllable surface porosity, it is feasible to develop a nanoscale system for targeted drug delivery with the diagnostic information encoded in the fluorophore.
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