Morphology linked to miscibility in highly amorphous semi-conducting polymer/fullerene blends

• Molecular miscibility determines residual fullerene in mixed polymer-rich phase.
• Molecular miscibility influences domain spacing in bulk heterojunction thin films.
• Fluorine substitution reduces molecular miscibility.

Molecular miscibility is a defining property of mixtures of electron-donating polymers and electron-accepting fullerenes used in the photoactive layer of bulk heterojunction (BHJ) organic solar cells. Even though miscibility of fullerene in the polymer is a commonly observed property, quantitative measurements have unknown connections with other morphological properties such as domain size and domain purity. By varying the amount of fullerene loading in BHJ thin films, we show that morphological properties are related to miscibility via straightforward relationships. In particular, miscibility influences the sensitivity of domain spacing to fullerene loading and determines the domain volume fractions and the residual fullerene content in the mixed polymer-rich phase in devices. Not only does this work show the relationships between miscibility and morphology, but it also highlights the general importance in determining miscibility levels in BHJ systems in order to target optimum morphologies and domain purities.

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