Abstract
In this thesis, we report that a "tree-like" dendrigraft ofpoly-L-Lysine (DGL) is able to form a multi-ligand complex with afluorescently labelled peptide, leading to the almost complete extinction ofthe optical signal that can be restored upon the introduction of heparin. This simple system allows, for the first time, the turn-ON fluorescent sensing of the anticoagulant in human blood at clinically relevant levels. Then, we demonstrate that this sensing ensemble can evolve toward a sensorarray. Depending on the loading of the indicator on the receptor, negatively charged glycosaminoglycans (GAGs) induce a positive or negative variation of the fluorescent signal as they displace the indicators from the receptor or they compact the indicators on the receptor’s surface, respectively. This unique strategy allows not only the blind identification of pure GAGs with a level of accuracy of 100 %, but also the differentiation of mixtures.We also report an original and simple methodology for the construction of three-dimensional structures of DGLs, and the subsequent investigation of their structural features using molecular dynamics simulations. This methodology relies on the encoding of the polymers’ experimental characterizations (i.e. degrees of polymerization, branchingratios, charges) into alphanumeric strings that are "readable" by the Ambersimulation package. This work opens avenues toward the in silico exploration of dendrigrafts and hyperbranched polymers.Finally, we developed ChemBrows, an in-house software that will significantly help scientists/teachers/ students to tame the flood of publications.Working as an enhanced RSS reader that integrates keyword-based filters anda machine-learning-based recommendation engine, ChemBrows is available onmultiple platforms as a free and open-source software at www.chembrows.com.