Exciton Transport in Singlet Fission Materials: A New Hare and Tortoise Story.

Abstract

Singlet fission is promising for redistributing the solar spectrum to overcome the Shockley-Queisser limit for single-junction solar cells using molecular materials. Despite recent experimental and theoretical advances in understanding the underlying mechanisms, how exciton transport is coupled to singlet fission dynamics is much less explored. In this Perspective, we examine exciton transport in singlet fission materials, highlighting the use of transient absorption microscopy (TAM) to track the population of different states in both spatial and temporal domains. In contrast to the conventional picture where singlet and triplet excitons migrate independently, TAM measurements of acene single crystals reveal cooperative transport between fast-moving singlet and slow-moving triplet excitons. Such cooperative transport is unique to singlet fission materials and allows hundreds of nanometers triplet migration on the nanosecond time scale, beneficial for solar cell applications. The transport of triplet pair intermediates and general criteria for achieving cooperative singlet-triplet transport are also discussed.