Fullerene-Dependent Miscibility in the Silole-Containing Copolymer PSBTBT-08

A high fullerene molecular miscibility of over 40 wt % is found in the copolymer poly((4,4-octyldithieno(3,2-b:2′,3′-d)silole)-2,6-diyl-alt-(2,1,3-benzothiadiazole)-4,7-diyl) (PSBTBT-08)a member of the PSBTBT low-bandgap polymer family that have produced power conversion efficiencies as high as 5.9% in solar cells. This observation suggests molecular miscibility plays a key role in the photovoltaic effect in this system. The level of miscibility is additionally measured to be highly dependent on the fullerene species with significant differences between C₆₀- and C₇₀-based fullerenes, highlighting a new parameter to be monitored and controlled when considering different fullerene moieties and species in organic solar cells. Surprisingly, a wide-angle X-ray scattering study reveals no significant crystallinity in the PSBTBT with octyl side chains, potentially the cause of low mobilities and in stark contrast to dodecyl and ethylhexyl PSBTBTs, which demonstrates the importance of the side chain in device morphology and performance.