Recently, it was reported that crystals of the organic material dithiophene-tetrathiafulvalene (DT-TTF) have a high field-effect charge carrier mobility of 1.4 cm(2)/(V x s). These crystals were formed by a simple drop-casting method, making this material interesting to investigate for possible applications in low-cost electronics. Here, organic single-crystal field-effect transistors based on materials related to DT-TTF are presented and a clear correlation between the crystal structure and the electrical characteristics is observed. The observed relationship between the mobilities in the different crystal structures is strongly corroborated by calculations of both the molecular reorganization energies and the maximum intermolecular transfer integrals. The most suitable materials described here exhibit mobilities that are among the highest reported for organic field-effect transistors and that are the highest reported for solution-processed materials.
The packing in molecular crystals is determined by intermolecular interactions. An understanding of these interactions would enable the design of systems exhibiting effective conductivity and superconductivity. By careful analysis of the shortest intermolecular interactions in the crystal combined with accurate ab‐initio calculatins it has been shown that CH…X and S…S are the two interactions most likely to influence the structures of these materials.
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