Investigating Plasmonic Structure-Dependent Light Amplification and Electronic Dynamics Using Advances in Nonlinear Optical Microscopy

Abstract

Our group has made several recent advances using single-particle nonlinear optical (NLO) microscopy techniques to examine nanostructure-specific plasmon-mediated interactions with electromagnetic energy. These efforts are directed toward the larger goal of optimizing the structure of photonic nanoparticle assemblies for the use and control of energy at the nanoscale. By combining statistical localization methods with second harmonic generation (SHG) imaging, nonlinear signal hot spots can be located within a plasmonic network with nanometer spatial accuracy. This experimental capability was applied to study electromagnetic lensing effects in plasmonic nanoparticle assemblies, with the efficiency of cascaded energy transfer through the network being determined by the resonantly excited plasmon mode. The polarization and time dependencies of the NLO signals were examined using a sequence of phase-locked broad bandwidth femtosecond laser pulses. The methodologies for generating, characterizing, and incorpora...