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  1. Hayashi, H.; Sobczuk, A.; Bolag, A.; Sakai, N.; Matile, S. “Antiparallel Three-Component Gradients in Double-Channel Surface Architectures” Chem. Sci. 2014, 5, 4610-4614

The synthesis of multicomponent surface architectures with a thus far inaccessible level of sophistication is accomplished, and the functional relevance of this unprecedented structural complexity is demonstrated. Co-axial channels of oligothiophenes and fullerenes for the transport of holes and electrons, respectively, are equipped with antiparallel-oriented redox gradients with up to three components that drive the charges apart after their generation with light. In the resulting photosystems, charge recombination decreases with each level of sophistication from 29% to 2%, approaching complete suppression. Photocurrents increase correspondingly, and thermal activation barriers decrease. Increasing turn-on voltages for dark current indicates that charges struggle to move backwards up gradients possessing increasing numbers of components. These results demonstrate that the application of the most complex lessons from nature to organic materials is possible and worthwhile, thus supporting curiosity-driven efforts to learn how to synthesize multicomponent architectures of the highest possible sophistication with the highest possible precision.

DOI: 10.1039/C4SC02092H 

open archive unige:41393 • pdf