Transport of Spin-Entangled Triplet Excitons Generated by Singlet Fission

Abstract

Singlet fission provides a promising route for overcoming the Shockley-Queisser limit in solar cells using organic materials. Despite singlet fission dynamics having been extensively investigated, the transport of the various intermediates in relation to the singlet and triplet states is largely unknown. Here we employ temperature-dependent ultrafast transient absorption microscopy to image the transport of singlet fission intermediates in single crystals of tetracene. These measurements suggest a mobile singlet fission intermediate state at low temperatures, with a diffusion constant of 36 cm²s^-1 at 5 K, approaching that for the free singlet excitons, which we attribute to the spin-entangled correlated triplet pair state ¹[TT]. These results indicate that ¹[TT] could transport with a similar mechanism as the bright singlet excitons, which has important implications in designing materials for singlet fission and spintronic applications.