A Ground-State Dual-Descriptor Strategy for Screening Efficient Singlet Fission Systems.

Abstract

Exploration of singlet fission (SF) materials is vital for enhancing the photoelectric conversion efficiency of photovoltaic devices, and the development of an effective screening means is in great demand. In this work, we for the first time propose a promising dual-descriptor strategy to predict the SF energetics (ΔESF) from ground-state electronic properties, the gap (GapHL) and exchange energy (KHL) between the highest occupied and lowest unoccupied molecular orbitals (HOMO and LUMO), where GapHL plays a dominant role and KHL acts as a correction. This strategy is statistically verified through exploring the effect of N-doping on the electronic/energetic properties of the N-doped tetracene derivatives and isomers. Several rules of thumb are suggested, and the reliability of this strategy is validated by comparison with experiments. This work proposes a novel strategy for exploring SF chromophores with insights into the SF energetics from ground-state properties and certainly has fundamental interest and generality in exploring efficient SF-capable materials.