Numerical simulations of ultrafast dynamics in plasmonic nanostructures

Abstract: Plasmonic effects in nanosized particles enhance the interaction between light and matter due to the localized surface plasmon resonance, with potential applications such as all-optical transistors and optical computers. Commonly, the dynamics of nanoparticles’ optical properties are assessed via pump-probe spectroscopy, where a plasmonic structure is exited by an initial laser, the pump. Thereafter a second, less intense laser, a probe, interacts with the now excited structure at a time delay. Through measurements of the probelight transmitted by the matter, the optical dynamics of the structure are monitored. Similar methodologies can potentially be used for other applications as well, such as all-optical switching. This study focuses on an implementation of a numerical finite element method model simulating a pump-probe experiment to predict the effects of different geometries and evaluate experimental data. The simulations are split into three parts. Initially, periodically spaced nanoparticles are excited by the pump laser. Then the model estimates the internal thermal dynamics of the excited nanoparticles and in turn, determines the change in complex permittivity. Lastly, the probe-matter interaction is modeled. To evaluate the model, a comparison with another model was performed. Furthermore, simulations of periodically spaced gold dimer nanoparticles in air were done to investigate how dimers affect transmitted light. For a probe light polarization rotated 45◦ against the axis parallel to the dimer, a change in rotation of 6◦ over 35 fs was induced by the pump, indicating a potential switching mechanism.