Abstract

The molecular organization at interfaces of organic semiconducting materials plays a crucial role in the performance of organic photovoltaics and field effect transistors. Vibrational sum-frequency generation (VSFG) was used to characterize the molecular orientation at interfaces of regioregular poly-3-hexylthiophene (rrP3HT). Polarization-selected VSFG spectra of the C═C stretch of the thiophene ring yield the orientation of the conjugated backbone of P3HT, which is directly relevant to the electronic properties at the interface. The molecular orientation at buried polymer–substrate interfaces was compared for films spin-cast on SiO2 and AlOX substrates, before and after thermal annealing at 145 °C. On SiO2, annealing results in the thiophene rings adopting a more edge-on orientation, tilting away from the surface plane by Δθ = +(3–10)°. In contrast, an opposite change is observed for films deposited on AlOx, Δθ = −(3–26)°, where annealing leads to a more face-on orientation of the thiophene rings of the...

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