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Pérovskites hybrides et ingénierie d'interface pour l'amélioration des dispositifs optoélectroniques

Abstract : The serious energy shortage and environmental pollution problems urge the development for renewable energies. Photovoltaic technologies as one of the most promising strategy have attracted extensive attention since middle of 20 century. Nowadays, perovskite solar cells lead the next-generation photovoltaic devices due to their superior photovoltaic properties. The certified record efficiencies for a single junction PSC and a 2-terminal OIHP/Si tandem solar cell have already reached 25.2% and 29.1% nowadays.In this thesis, we have investigated OIHP solar cells in terms of interface control and composition engineering. An introduction of our research background is written in Chapter I. Basic semiconductor knowledges, working principle of photovoltaic devices and a bibliographic review are given in this chapter. Besides, we also provided a brief introduction about ultra-violet (UV) photodetectors (PDs) and explained several important parameters for UV PDs.In Chapter II, we have first studied the effect of modifying TiO2 layers by various organic acid molecules with a dipole moment varying in a large range. The acid modifiers adsorption has been then thoroughly investigated by a combined experimental and theoretical approach. We have then designed and fabricated a solid-state nanostructured UV-A photodetector based on the TiO2/Spiro-OMeTAD p-n heterojunction. Reliable study of the effect of interfacial acid modifiers on the PD response was provided in this Chapter.In Chapter III, we have demonstrated that the engineering of the interface between perovskite and titania is important to get highly efficient perovskite solar cells. We have shown that in high efficiency triple cation PSCs, the chloride-functionalized benzoic acid molecule provides a significant beneficial effect. Our experimental and theoretical investigations emphasize that CBA SAMs at the oxide/perovskite interface is beneficial for the structural continuity, the trap state reduction and for the global quality of the perovskite.In Chapter IV, we have developed the use of methyl ammonium chloride as an additive in rather low concentration mixed organic cation precursor solutions. MACl is shown to mediate the growth of the layers. The resulting films were uniform, compact, with no pinholes and made of remarkably large size perovskite crystal grains. To further increase the PCE of the solar cells, a treatment with a PEAI solution has been implemented. This treatment, without any thermal annealing step, leads to the spontaneous formation of (PEA)2PbI4 perovskite at the surface. This buffer layer has been shown to favor a fast transfer of the holes towards the HTL and to reduce the recombination at the perovskite/HTL interface. Overall, the optimized devices had a PCE higher than 22.1%.In Chapter V, BEI based mixed-dimensional (MD) OIHPs were employed as a light absorber layer due to their excellent stability against moisture. We have systematically studied the properties of the so-called MD-OIHP solar cells. A series of perovskite films with molecular formula of BE2FAn-1PbnI3n+1 (n = 1, 2, 3, 5, 9, and ∞) were fabricated. The optimized solar cell kept the black phase for 104 days in ambient environment, while the stable Cs8FAMA cell just kept it for 1 day.
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Tao Zhu. Pérovskites hybrides et ingénierie d'interface pour l'amélioration des dispositifs optoélectroniques. Chimie analytique. Université Paris sciences et lettres, 2020. Français. ⟨NNT : 2020UPSLC020⟩. ⟨tel-03551362⟩

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