RESUMO
The process of spontaneous emission can be dramatically modified by optical microstructures and nanostructures. We have studied the modification of fluorescence dynamics using a variable thickness polymer spacer layer fabricated using layer-by-layer self-assembly with nanometer accuracy. The change in fluorescence lifetime with spacer layer thickness agrees well with theoretical predictions based on the modified photonic density of states (PDOS), and yields consistent values for the fluorophores' intrinsic fluorescence lifetime and quantum yield near a dielectric as well as a plasmonic interface. Based on this observation, we further demonstrate that self-assembled fluorophores can be used to probe the modified PDOS near optical microstructures and nanostructures.
RESUMO
We have demonstrated large enhancements of the effective second-order nonlinear susceptibility (chi(2)) of ionic self-assembled multilayer (ISAM) films, causing a film with just 3 bilayers to be optically equivalent to a 700-1000 bilayer film. This was accomplished by using nanosphere lithography to deposit silver nanoparticles on the ISAM film, tuning the geometry of the particles to make their plasmonic resonances overlap the frequency of optical excitation. An enhancement in the efficiency of second harmonic generation (SHG) by as much as 1600 times was observed. Even though this is already a large value, we suggest that further refinements of the techniques are expected to lead to additional enhancements of similar or larger magnitude.
