Importance of 2D Conjugated Side Chains of Benzodithiophene-Based Polymers in Controlling Polymer Packing, Interfacial Ordering, and Composition Variations of All-Polymer Solar Cells

• Published in: Chemistry of materials Vol. 29; no. 21; pp. 9407 - 9415
• Main Authors: Lee, Changyeon, Giridhar, Thota, Choi, Joonhyeong, Kim, Seonha, Kim, Youngwoong, Kim, Taesu, Lee, Wonho, Cho, Han-Hee, Wang, Cheng, Ade, Harald, Kim, Bumjoon J
• Format: Journal Article
• Language: English
• Published: American Chemical Society 14.11.2017
• ISSN: 0897-4756; 1520-5002
• DOI: 10.1021/acs.chemmater.7b03495

We delineate the important role of 2D conjugated alkylthiophene side chains of polymers in manipulating the molecular orientation and ordering at the polymer donor/polymer acceptor (P D/P A) interface as well as the composition variations in the blend active layer of all-polymer solar cells (all-PSCs). To systematically investigate the impact of 2D conjugated side chains on the performance of all-PSCs, we synthesized a series of poly­(benzo­[1,2-b:4,5-b̀]-dithiophene-thieno­[3,4-c]­pyrrole-4,6-dione) (PBDTTPD) polymer donors with different contents of alkoxy and alkylthiophene side chains, from 0 to 100% (PBDT-TPD (P1, 100% alkoxy side chain), PBDTT0.29-TPD (P2), PBDTT0.59-TPD (P3), PBDTT0.76-TPD (P4), and PBDTT-TPD (P5, 100% alkylthiophene side chain). The P1–P5 polymer donors produced similar PCEs of ∼6% in fullerene-based PSCs. In contrast, for the all-PSC systems, the changes in the side chain composition of the polymers induced a strong increasing trend in the power conversion efficiencies (PCEs), from 2.82% (P1), to 3.16% (P2), to 4.41% (P3), to 5.32% (P4), and to 6.60% (P5). The significant increase in the PCEs of the all-PSCs was attributed mainly to improvements in the short-circuit current density (J SC) and fill factor (FF). The 2D conjugated side chains promoted localized molecular orientation and ordering relative to the P D/P A interfaces and improved domain purity, which led to enhanced exciton dissociation and charge transport characteristics of the all-PSCs. Our observations highlight the advantage of incorporating 2D conjugated side chains into polymer donors for producing high-performance all-PSC systems.