Electron and Lattice Heating Contributions to the Transient Optical Response of a Single Plasmonic Nano-Object

The sudden absorption of light by a metal nanoparticle launches a series of relaxation processes (internal thermalization, acoustic vibrations, and cooling) which induce a transient modification of its optical response. In this work, the transient optical response associated with the internal thermalization of a single gold nanodisk (occurring on a few picoseconds time scale) was quantitatively investigated by time-resolved spectroscopy experiments, and the measured signals were compared with a model accounting for the effects of both electron and ionic lattice heating. We show that experimental time-resolved signals at delays posterior to nanodisk excitation and electron gas thermalization can be simply interpreted as a combination of electron and lattice temperature evolutions, with probe wavelength-dependent weights. This demonstrates the possibility to selectively probe the electronic or lattice dynamics, through the choice of specific probe wavelengths. Additionally, the time-dependent spectral shape of transient extinction cross-section changes is shown to be successively dominated by the effects of electron and lattice heating, which present distinct spectral signatures.