Thèse de doctorat
Résumé : Systems chemistry aims at studying and developing "smart" materials displaying reactivity to external stimuli, metabolism, self-repair abilities and self-replication properties. These features constitute the principal characteristics of living systems that smart materials tend to mimic. The synthesis strategies of these materials are still in their infancy, and identifying the mechanisms underlying emergent phenomena could lead to a better control and use of these behaviours in the synthesis of new materials. The complex dynamics of biological systems usually arises from the coupling of compartmentalised units in which nonlinear chemical reactions take place. In this thesis, we are interested in the complex dynamics emerging from such compartmentalisation of a reactive system. First, we analyse the impact of fluctuations of concentration on the dynamics of a chemical oscillatory reaction, namely the Belousov-Zhabotinsky reaction. We show that oscillations are more robust against fluctuations than other behaviours generated by the reaction (birhythmicity, chaos, ...) and highlight different mechanisms by which oscillations can arise from fluctuations. Then, we study a model for chemical chaos, the so-called Willamowsky-Rössler model, in which we incorporate fluctuations and crowding effects. Fluctuations have a destructive effect on chaotic dynamics but when the reaction takes place on a surface where the different species can diffuse and react, a synergy develops between fluctuations, crowding effects and the mobility of the particles. This synergy enhances the re-emergence of chaos and the development of new behaviours. Finally, we show throughout different modelling approaches that compartmentalisation effects play a central role in the intracellular calcium dynamics and emphasise how microscopic properties of the system shape the global behaviour of this system. Compartmentalised nonlinear dynamics thus offer a wide range of future prospects for the synthesis of smart materials and fosters the development of nanoreactors based on these properties.