Propriétés statiques et dynamiques électroniques ultrarapides dans les molécules carbonées, du régime linéaire au non-linéaire

Abstract : The works presented in this thesis are part of project MUSES (MUltiscale Electron Spectroscopy) which consist in a combined experimental and theoretical approach on the study of electronic dynamics in molecules over a large time range. They concentrate particularly on electrons dynamics in carbonates molecules at the femtosecond and attosecond timescales. In order to understand processes occurring in those complex systems, it is necessary to study them in linear excitation regime as well as non linear one. Indeed, many electron dynamics theoretical models, valid in case of atoms or diatomic systems collapse in the case of polyatomic molecules. Moreover, the access to ultrafast light sources now allows to probe multielectronic processes and confront experimental results to theoretical calculations. Model systems C60, PAHs (Naphtalene, Anthracene and Pyrene) as well as DNA/RNA bases (pyrimidic bases Cytosine, Thymine, Uracile) have been the principal objects of study in that purpose. Experiments have been done in angularly resolved photoelectron spectroscopy and ionisation products mass spectroscopy, under XUV (10-30 eV) weak field synchrotron excitation, intense near infrared (I 1013 W/cm2) excitation as well as on a pump-probe XUV-IR laser beamline that give access to a hundred attosecond time resolution. With help of those tools, we evidenced and modeled the influence of the surface plasmon resonance of C60 at 20 eV in its photoionization dynamics at the attosecond timescale. We identified the population of Rydberg states during multiphoton ionisation of DNA/RNA bases similar for all the bases. This constraints theoretical models about non linear response of complex system under those excitation conditions. Finally we have been able to observe non adiabatic dynamics (electrons-nucleus couplings at a few tens of femtoseconds timescale) that appear consecutively of multielectronic excitation and ionization processes (shake-up mechanism)
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Thomas Barillot. Propriétés statiques et dynamiques électroniques ultrarapides dans les molécules carbonées, du régime linéaire au non-linéaire. Autre [cond-mat.other]. Université Claude Bernard - Lyon I, 2013. Français. ⟨NNT : 2013LYO10156⟩. ⟨tel-01128292⟩

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