Nanoscale Correlation between Exciton Dissociation and Carrier Transport in Silole-Containing Cyclopentadithiophene-Based Bulk Heterojunction Films

Abstract

Understanding the effects of conjugated polymer structures on exciton lifetimes and morphologies within bulk heterojunction (BHJ) films is a necessary step toward the development of better organic solar cells. Studying the impact of a polymer's structure on the optical, morphological, and performance characteristics of a device can lead to advances in the design of new polymers. In this study, we synthesized carbon- and silicon-bridged cyclopentadithiophene- (CPDT-) based polymers and determined their photophysical properties and morphologies by measuring the exciton lifetime distributions in their BHJ films The silicon-bridged CPDT-based polymer/[6,6]-phenyl-C(61)-butyric acid methyl ester (PCBM) BHJ exhibited a higher degree of luminescence quenching, suggesting that thermodynamically favorable mixing on the molecular scale and nanoscale phase separation occurred simultaneously in the blend film. We attribute this favorable morphology to the presence of strong pi-pi stacking in the silicon-bridged CPDT-based polymers. Under AM 1.5 G illumination (100 mA cm(-2)), a device incorporating the silicon-bridged CPDT-based polymer and PCBM (1:2, w/w) gave an overall power conversion efficiency of 3.5% with a short-circuit current of 9.0 mA cm(-2), an open-circuit voltage of 0.72 V, and a fill factor of 53.6%.