Polymerized-Small-Molecule Acceptors Featuring Siloxane-Terminated Side Chains for Mechanically Robust All-Polymer Solar Cells.

Flexible and stretchable organic solar cells (OSCs) show great promise in wearable and stretchable electronic applications. However, current high-performance OSCs consisting of polymer donors (PDs) and small-molecule acceptors (SMAs) face significant challenges in achieving both high power conversion efficiency (PCE) and excellent stretch-ability. In this study, we synthesized a new polymerized-small-molecule acceptor (P-SMA) PY-SiO featuring siloxane-terminated side chains and compared its photovoltaic and mechanical performance to that of the reference PY-EH with ethylhexyl-terminated side chains. We found that the incorporation of siloxane-terminated side chains in PY-SiO enhanced the molecular aggregation and charge transport, leading to an optimized film morphology. The resultant of all-polymer solar cells (all-PSCs) based on PBDB-T/PY-SiO showed a higher PCE of 12.04% than the PY-EH-based one (10.85%). Furthermore, the siloxane-terminated side chains also increased the interchain distance and provided a larger free volume for chain rotation and reconfiguration, resulting in a higher film crack-onset strain (COS: 18.32% for PBDB-T/PY-SiO vs 11.15% for PBDB-T/PY-EH). Additionally, the PY-SiO-based stretchable all-PSCs exhibited an impressive PCE of 9.8% and retained >70% of its original PCE even under a substantial 20% strain, exceeding the performance of the PY-EH-based stretchable all-PSCs. Our result suggests the great potential of the siloxane-terminated side chain for achieving high-performance and stretchable OSCs.