Wavelength-Orthogonal Optodynamics to Overcome the Statistical Limitations of Interfacial Photopolymerizations

Presently, error correction of covalent bonds for the controlled synthesis of ordered multidimensional materials is largely restricted to thermal methods, which oftentimes require harsh reaction conditions. This limitation affects interfacial applications, for example, in emulsions that are central to many industrial applications in energy, healthcare, or foods. Herein, we introduce wavelength-orthogonal optodynamics, which enables photoinduced error correction and provides a mild alternative to conventional dynamic covalent chemistry. We demonstrate that the dynamic interplay between two wavelengths (440 and 370 nm) can be harnessed for the preferential cleavage of suboptimal linkages to induce major structural improvements in interfacial polymer shells of emulsions. This overwrites the inherent statistical limitations of conventional photopolymerizations, which traditionally result in highly heterogeneous and defective structures. Overall, the work exemplifies the opportunities of wavelength-orthogonal optodynamic chemistry for the generation and modification of organic materials and highlights the prospect of it to areas previously inaccessible to dynamic covalent synthesis.