Bending and pinching of three-phase stripes: From secondary instabilities to morphological deformations in organic photovoltaics.

Abstract

Optimizing the properties of the mosaic nanoscale morphology of bulk heterojunction (BHJ) organic photovoltaics (OPV) is not only challenging technologically but also intriguing from the mechanistic point of view. Among the recent breakthroughs is the identification and utilization of a three-phase (donor-mixed-acceptor) BHJ, where the (intermediate) mixed phase can inhibit mesoscale morphological changes, such as phase separation. Using a mean-field approach, we reveal and distinguish between generic mechanisms that alter, through transverse instabilities, the evolution of stripes: the bending (zigzag mode) and the pinching (cross-roll mode) of the donor-acceptor domains. The results are summarized in a parameter plane spanned by the mixing energy and illumination, and show that donor-acceptor mixtures with higher mixing energy are more likely to develop pinching under charge-flux boundary conditions. The latter is notorious as it leads to the formation of disconnected domains and hence to loss of charge flux. We believe that these results provide a qualitative road map for BHJ optimization, using mixed-phase composition and, therefore, an essential step toward long-lasting OPV. More broadly, the results are also of relevance to study the coexistence of multiple-phase domains in material science, such as in ion-intercalated rechargeable batteries.