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Towards two-dimensional organo-metallic molecular architecture via interface chemistry

Abstract : Compared to inorganic two-dimensional materials (e.g. graphene, transition metal dichalcogenides), organic two-dimensional materials are all synthetic materials, that additionally have a more complex structure inherited from their building blocks. A richer set of properties is for this reason expected from them, and their production should be unexpensive.In this thesis manuscript we present our work on two strategies toward the formation of such organic two-dimensional, or at list ultrathin organic sheet materials. These strategies rely on interfacial chemistry, on one hand at the vacuum/solid interface, and on the other hand the liquid/liquid interface. The first strategy is based on surface science tools (scanning tunneling microscopy, X-ray photoemision and absorption near-edge spectroscopies, density functional theory) and addressed triphenylene derivative molecules experiencing chemical modifications on the well-defined (111) surface of copper. Although we did not yet manage to prepare an extended two-dimensional material in this system, we discovered that the molecules get catalytically oxidized and concomitantly change in shape, surface organization, and interaction with the substrate. We establish that the fully-oxidized molecules are stronger electron acceptor than most known molecules. The second strategy is based on in-solution synthesis and more versatile characterization (UV-visible and Raman spectroscopies, optical and electron microscopies). It exploits dynamic imine bond chemistry starting from ruthenium(arene) monomers, to form polymeric organometallic nanosheets that are conveniently manipulated and can for instance be suspended across membrane.
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Ana Cristina Gomez Herrero. Towards two-dimensional organo-metallic molecular architecture via interface chemistry. Materials Science [cond-mat.mtrl-sci]. Université Grenoble Alpes, 2019. English. ⟨NNT : 2019GREAY068⟩. ⟨tel-02633111⟩

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