Highly mobile charge-transfer excitons in two-dimensional WS2/tetracene heterostructures

Abstract

Charge-transfer (CT) excitons at heterointerfaces play a critical role in light to electricity conversion using organic and nanostructured materials. However, how CT excitons migrate at these interfaces is poorly understood. We investigate the formation and transport of CT excitons in two-dimensional WS2/tetracene van der Waals heterostructures. Electron and hole transfer occurs on the time scale of a few picoseconds, and emission of interlayer CT excitons with a binding energy of ~0.3 eV has been observed. Transport of the CT excitons is directly measured by transient absorption microscopy, revealing coexistence of delocalized and localized States. Trapping-detrapping dynamics between the delocalized and localized States leads to stretched-exponential photoluminescence decay with an average lifetime of ~2 ns. The delocalized CT excitons are remarkably mobile with a diffusion constant of ~1 cm2 s−1. These highly mobile CT excitons could have important implications in achieving efficient charge separation.