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Étude des phénomènes thermiques ultrarapides dans les nanostructures plasmoniques

Abstract : Thermoplasmonics is a branch of plasmonics exploiting thermal phenomena in metallic structures. Long regarded as problematic, Joule losses due to the absorption of light by metallic nanoparticles are now considered as a starting point for many applications: thermal nanosources in medicine, magnetic recording, chemical catalysis, thermotronics or energy conversion.The use of femtosecond lasers on plasmonic structures, allows the creation of spatially confined nanosources of heat reaching very high electronic temperatures compared to the temperature of the atomic lattice. The absorption by a metal of a pulse of energy can be described in three main steps. Firstly, an absorption of photons by the electrons of the metal increases the electron energy on the scale of a hundred femtoseconds with electronic temperatures that can reach thousands of Kelvin, while the lattice temperature remains almost constant. Then, a second step, in which the electron-phonon interactions transmit the energy absorbed by the electrons to the grid, allowing the electrons and phonons to reach equilibrium. Finally, the energy is dissipated into the substrate surrounding the metal by thermal conduction.Many models exist in the literature to describe the non-equilibrium between electrons and phonons. However, a rigorous and quantitative comparison with experimental data is lacking to validate or invalidate these models. This was the main objective of this study.To study these phenomena, I used a pump-probe experiment where the pump allows an ultra-fast heating of the sample which causes a change in the permittivity of the metal. The probe beam then allows to measure the variations in the reflection and transmission spectrum, caused by the change in permittivity.I set up a numerical code allowing to model the temperature evolution in a 3D mesh of a structure composed of dielectric and metallic elements. This thermal model takes into account the various energy transport phenomena in a metal such as electron-phonon coupling, electron and phonon thermal conduction and ballistic displacement of non-thermalized electrons. Then, via a model of permittivity as a function of temperature taking into account the interband and intraband transitions, this model was coupled to an optical model to simulate the evolution of the optical spectra of a structure as a function of its temperature in order to be able to confront this numerical model with the experimental results by data fitting.This numerical model has been validated on numerous pump-probe experiments carried out on gold films of various thicknesses and gold nanostructure arrays on glass or gold film. We were able to show that, among the very large number of optical and thermal parameters involved in the model, all these experimental data could be adjusted using a very small number of free parameters, thus confirming the robustness of the model. Finally, this model was used to design and optimize samples allowing the experimental demonstration of heat propagation on scales of a few hundred nanometers within a gold nanostructure.
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Paul Bresson. Étude des phénomènes thermiques ultrarapides dans les nanostructures plasmoniques. Thermique [physics.class-ph]. Université Paris-Saclay; Université de Sherbrooke (Québec, Canada), 2020. Français. ⟨NNT : 2020UPAST005⟩. ⟨tel-03129996⟩

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