Second-Order Photoinduced Reflectivity for Retrieval of the Dynamics in Plasmonic Nanostructures

[Image: see text] Measuring the change in reflectivity (ΔR) using the traditional pump–probe approach can monitor photoinduced ultrafast dynamics in matter, yet relating these dynamic to physical processes for complex systems is not unique. By applying a simple modification to the classical pump–probe technique, we simultaneously measure both the first and second order of ΔR. These additional data impose new constraints on the interpretation of the underlying ultrafast dynamics. In the first application of the approach, we probe the dynamics induced by a pump laser on the local-surface plasmon resonance (LSPR) in gold nanoantennas. Measurements of ΔR over several picoseconds and a wide range of probe wavelengths around the LSPR peak are followed by data fitting using the two-temperature model. The constraints, imposed by the second-order data, lead us to modify the model and force us to include the contribution of nonthermalized electrons in the early stages of the dynamics.