Photoresponse of an Organic Semiconductor/Two-Dimensional Transition Metal Dichalcogenide Heterojunction

We study the optoelectronic properties of a type-II heterojunction (HJ) comprising a monolayer of the transition metal dichalcogenide (TMDC), WS2, and a thin film of the organic semiconductor, 3,4,9,10-perylene tetracarboxylic dianhydride (PTCDA). Both theoretical and experimental investigations of the HJ indicate that Frenkel states in the organic layer and two-dimensional Wannier-Mott states in the TMDC dissociate to form hybrid charge transfer excitons at the interface that subsequently dissociate into free charges that are collected at opposing electrodes. A photodiode employing the HJ achieves a peak external quantum efficiency of 1.8 +/- 0.2% at a wavelength of 430 +/- 10 nm, corresponding to an internal quantum efficiency (IQE) as high as 11 +/- 1% in these ultrathin devices. The photoluminescence spectra of PTCDA and PTCDA/WS2 thin films show that excitons in the WS2 have a quenching rate that is approximately seven times higher than in PTCDA. This difference leads to strong wavelength dependence in IQE.