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Novel ethyladamantyl solubilization side groups were found to induce π–π interactions between the conjugated cores through adamantyl–adamantyl stacking in soluble diketopyrrolopyrrole (DPP) derivatives. The closeness of the DPP cores amplifies charge transfer in the material, as far as the π–π interaction is a dominant charge-hopping pathway. As a result, tenfold enhancement of hole mobilities exceeding those obtained for insoluble derivatives was reached. Moreover, due to high crystallinity and co-planarity of the conjugated cores, electron transfer was preserved with a mobility of 0.2 cm2 V−1 s−1 for dithiophene-DPP. At the same time, the material remained soluble, which is a significant advantage for purification and processing. This approach can be universally applied for many types of semiconducting organic materials containing the imide motif, where solubilization is achieved by side-group substitution.

Weak localization describes a metallic system, where due to the presence of disorder the electrical transport is governed by inelastic electron relaxation. Therefore the theory defines a threshold of spatial and of energetic disorder, at which a metal-insulator transition takes place. To achieve a metallic state in an inherently disordered system such as a conductive polymer, one has to overcome the threshold of localization. In this work we show that the effective suppression of disorder is possible in solution-processible poly(3,4-ethylenedioxythiophene)-poly(styrene sulfonate). We grow polymer films under optimized conditions allowing self-organization in solution. Interestingly, we find the requisite threshold, at which the system becomes finally metallic. We characterize the transition using a complementary morphology and magneto-electrical transport study and find coherent electron interactions, which emerge as soon as local order exceeds the macromolecular dimensions. These insights can be used for discrete improvement in the electrical performance, in particular for tailoring conductive polymers to alternative metal-like conductors.