Direct quantification of the plasmon dephasing time in ensembles of gold nanorods through two-dimensional electronic spectroscopy†

Abstract

In this study, we used two-dimensional electronic spectroscopy to examine the early femtosecond dynamics of suspensions of colloidal gold nanorods with different aspect ratios. In all samples, the signal distribution in the 2D maps at this timescale shows a distinctive dispersive behavior, which can be explained by the interference between the exciting field and the field produced on the nanoparticle's surface by the collective motion of electrons when the plasmon is excited. Studying this interference effect, which is active only until the plasmon has been dephased, allows for a direct estimation of the dephasing time of the plasmon of an ensemble of colloidal particles. Our findings provide insight into the fundamental behavior of plasmonic states and highlight the potential of two-dimensional electronic spectroscopy in uncovering ultrafast and coherent optical phenomena at the nanoscale.