Precision Plasmonics with Monomers and Dimers of Spherical Gold Nanoparticles: Nonequilibrium Dynamics at the Time and Space Limits
Monomers and dimers of spherical gold nanoparticles (NPs) exhibit highly uniform plasmonic properties at the single-particle level due to their high structural homogeneity (precision plasmonics). Recent investigations in precision plasmonics have largely focused on static properties using conventional techniques such as transmission electron microscopy and optical dark-field microscopy. Here in this Feature Article, we first highlight the application of femtosecond time-resolved electron diffraction for monitoring the nonequilibrium dynamics of spherical gold NPs after ultrafast optical excitation. The analysis of the transient diffraction patterns allows us to directly obtain quantitative information on the incoherent excitation of the lattice, that is, heating upon electron–lattice equilibration, as well as on the development of strain due to lattice expansion on picosecond time scales. The controlled assembly of two spherical gold NPs into a dimer with a few nanometers gap leads to unique optical properties. Specifically, extremely high electric fields (hot spot) in the gap are generated upon resonant optical excitation. Conventional optical microscopy cannot spatially resolve this unique hot spot due to the optical diffraction limit. We therefore employed nonlinear photoemission electron microscopy to visualize hot spots in single dimers of spherical gold NPs. A quantitative comparison of different single dimers confirms the homogeneity of the hot spots on the single-particle level. Finally, overall, these initial results are highly encouraging because they pave the way to investigate nonequilibrium dynamics in highly uniform plasmonic nanostructures at the time and space limits.