Design of Multilayered Nanostructures and Donor–Acceptor Interfaces in Solution-Processed Thin-Film Organic Solar Cells


  • This work was partly supported by a Grant-in-Aid for Young Scientists (B) (no. 18750100), the 21st Century COE program (COE for a United Approach to New Materials Science), and Special Coordination Funds for Promoting Science and Technology from the Ministry of Education, Culture, Sports, Science, and Technology of Japan, and by the Integrative Industry–Academia Partnership (IIAP) project including Kyoto University, Nippon Telegraph and Telephone Corporation, Pioneer Corporation, Hitachi, Ltd., Mitsubishi Chemical Corporation, and Rohm Co., Ltd.


Multilayered polymer thin-film solar cells have been fabricated by wet processes such as spin-coating and layer-by-layer deposition. Hole- and electron-transporting layers were prepared by spin-coating with poly(3,4-ethylenedioxythiophene) oxidized with poly(4-styrenesulfonate) (PEDOT:PSS) and fullerene (C60), respectively. The light-harvesting layer of poly-(p-phenylenevinylene) (PPV) was fabricated by layer-by-layer deposition of the PPV precursor cation and poly(sodium 4-styrenesulfonate) (PSS). The layer-by-layer technique enables us to control the layer thickness with nanometer precision and select the interfacial material at the donor–acceptor heterojunction. Optimizing the layered nanostructures, we obtained the best-performance device with a triple-layered structure of PEDOT:PSS|PPV|C60, where the thickness of the PPV layer was 11 nm, comparable to the diffusion length of the PPV singlet exciton. The external quantum efficiency spectrum was maximum (ca. 20%) around the absorption peak of PPV and the internal quantum efficiency was estimated to be as high as ca. 50% from a saturated photocurrent at a reverse bias of −3 V. The power conversion efficiency of the triple-layer solar cell was 0.26% under AM1.5G simulated solar illumination with 100 mW cm−2 in air.