Ultrashort laser irradiation of gold nanorods in an aqueous medium: photo-generating processes of biomedical relevance

Gold nanoparticles exhibit specific optical properties thanks to surface plasmon resonance. Laser irradiation close to their resonance frequency induces two main effects: a high absorption of the electromagnetic energy and an enhancement of the electromagnetic field in their close vicinity. In addition, gold is biocompatible. These three features have made them extremely useful for a number of light-triggered biomedical applications. In this field, gold nanorods (AuNRs) specifically show promise. Indeed, their resonance frequency can be tuned by changing their aspect ratio in order to match the window where biological media are relatively transparent (650-1350 nm). Their resonance then exhibits a high quality factor. As a result, light irradiation of AuNRs triggers various complex biological effects, especially when intense, ultrashort pulses are used. Nevertheless, the physics of irradiated AuNRs in aqueous media is only properly understood in more simple situations. That is why this thesis aims at reaching a better understanding of these multiphysics in biologically relevant irradiation conditions. It provides theoretical, numerical and experimental pieces of information about the transient optical response, the dynamics of energy transfer, the plasmon-assisted plasma generation, the photoluminescence and the production of reactive oxygen species. Each of these processes has biological or biomedical impact. Analyzing the underlying mechanisms reveals above all the major role of hot electrons in the ultrashort regime. (author)