The spatially controlled functionalization of surface is currently widely investigated for several applications. Two techniques could be used to prepare such micropatterns. The first one is a photopolymerization from the surface whereas it is also possible to couple polymers onto surfaces by efficient ligation methods. Since ten years, we are working on the development of light-sensitive alkoxyamines as a efficient method to generate alkyl and nitroxide radicals with both temporal and spatial control. The position of the chromophore is a key parameter for its use. If located on the nitroxide moiety, it will allow to perform Nitroxide Mediated Photopolymerization (NMP2). Using first mask stereolithography, we showed that reinitiation of a polymerization from a surface prepared using a first monomer could occur and that patterns with another monomer having different properties could be obtained.<br/>In this study, we demonstrate the possibility of generating arbitrary polymer microstructures covalently linked to a first polymer layer by laser direct writing. In addition to the proof-of-concept and examples of achievable structures, including multichemistry patterns and 3D structures, this paper aims at investigating the physicochemical phenomena involved under such conditions. In particular, the parameters influencing the repolymerization process are considered, and special attention is paid to the study of the impact of oxygen on the spatial control of the polymerization. Such work opens many possibilities towards the fabrication of on-demand high-resolution (multi)functional polymer micro- and nanostructures.

Laser direct writing of arbitrary complex polymer microstructures by nitroxide-mediated photopolymerization

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ACS Fall 2022

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