Impact of dark excitons on Förster-type resonant energy transfer between dye molecules and atomically thin semiconductors

Abstract

Interfaces of dye molecules and two-dimensional transition metal dichalcogenides (TMDCs) combine strong molecular dipole excitations with high carrier mobilities in semiconductors. F\"orster type energy transfer is one key mechanism for the coupling between both constituents. We report microscopic calculations of a spectrally resolved F\"orster induced transition rate from dye molecules to a TMDC layer. Our approach is based on microscopic Bloch equations which are solved self-consistently together with Maxwell's equations. This approach allows to incorporate the dielectric environment of a TMDC semiconductor, sandwiched between donor molecules and a substrate. Our analysis reveals transfer rates in the meV range for typical dye molecules in closely stacked structures, with a nontrivial dependence of the F\"orster rate on the molecular transition energy resulting from unique signatures of dark, momentum forbidden TMDC excitons.