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The development of semicrystalline polymer semiconductors with field-effect mobilities comparable to or even exceeding those of amorphous silicon has exposed limitations of describing charge transport in these materials with disorder-based models developed originally for more disordered, lower mobility polymers. Here, we show that the charge carrier density and temperature dependence of the field-effect electron mobility and Seebeck coefficient in the semicrystalline polymer P(NDI2OD-T2) with varying degrees of crystallinity are incompatible with a description of charge transport being limited by energetic disorder effects. We provide instead direct evidence of low disorder, narrow band conduction. A spatially inhomogeneous density of states and the inclusion of short range electron–electron interactions allow to consistently explain both the measured mobility and Seebeck coefficient. These results provide a rationale for improving thermoelectric efficiency of polymer semiconductors via increasing the extension of the crystalline domains.In order to develop the next generation of semiconductor devices it is important to better understand the fundamental physics of materials other than silicon. The authors develop a theoretical approach to describe the charge transport properties of polymer-based semiconductors by focusing on features related to their crystallographic properties.

communications physics

On the manifestation of electron-electron interactions in the thermoelectric response of semicrystalline conjugated polymers with low energetic disorder