Rational molecular engineering towards efficient heterojunction solar cells based on organic molecular acceptors

The selection of photoactive layer materials for organic solar cells (OSCs) is essential for the photoelectric conversion process. It is well known that chlorophyll is an abundant pigment in nature and is extremely valuable for photosynthesis. However, there is little research on how to improve the efficiency of chlorophyll-based OSCs by matching chlorophyll derivatives with excellent non-fullerene acceptors to form heterojunctions. Therefore in this study we utilize a chlorophyll derivative, Ce 6 Me 3 , as a donor material and investigate the performance of its heterojunction with acceptor materials. Through density functional theory, the photoelectric performances of acceptors, including the fullerene derivative PC 71 BM and the terminal halogenated non-fullerene DTBCIC series, are compared in detail. It is found that DTBCIC-Cl has better planarity, light absorption, electron affinity, charge reorganization energy and charge mobility than others. Ce 6 Me 3 has good energy level matching and absorption spectral complementarity with the investigated acceptor molecules and also shows good electron donor properties. Furthermore, the designed Ce 6 Me 3 /DTBCIC interfaces have improved charge separation and reorganization rates ( K CS / K CR ) compared with the Ce 6 Me 3 /PC 71 BM interface. This research provides a theoretical basis for the design of photoactive layer materials for chlorophyll-based OSCs.