Promotion of Fast and Efficient Singlet Fission Process of PDI Dimers by Selenium Substitution

Singlet fission (SF) is a triplet generation mechanism capable of turning a singlet exciton into two triplet excitons. It has the potential to enhance the power conversion efficiency of single-junction solar cells. Perylene diimides (PDIs) are a class of dye molecules with photovoltaic properties and are beginning to receive more and more attention due to their potential for SF. Here, we report a selenium-substituted PDI dimer, Se-PDI-II, and we studied its SF mechanism by using steady-state, transient absorption, and time-resolved photoluminescence spectroscopy. Compared with the unsubstituted dimer PDI-II, we found that the introduction of selenium atoms can suppress excimer emission during the SF process, showing much higher SF efficiency and triplet yield.