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The rational assembly of monomers, in principle, enables the design of aspecific periodicity of polymeric frameworks, leading to a tailored set ofelectronic structure properties in these solid-state materials. The furtherdevelopment of these emerging systems requires a combination of bothexperimental and theoretical studies. Here, we investigated the electronicstructures of two-dimensional polymeric frameworks based on triazine andbenzene rings, by means of electrochemical techniques. The experimental densityof states was obtained from quasi-open-circuit voltage measurements throughgalvanostatic intermittent titration technique, which we show to be inexcellent agreement with first principles calculations performed for two andthree-dimensional structures of these polymeric frameworks. These findingssuggest that the electronic properties do not only depend on the number ofstacked layers but also on the ratio of the different aromatic rings.

Polymeric Frameworks as Organic Semiconductors with Controlled Electronic Properties