Near-Unity Efficiency Energy Transfer from Colloidal Semiconductor Quantum Wells of CdSe/CdS Nanoplatelets to a Monolayer of MoS₂.

Abstract

A hybrid structure of the quasi-2D colloidal semiconductor quantum wells assembled with a single layer of 2D transition metal dichalcogenides offers the possibility of highly strong dipole-to-dipole coupling, which may enable extraordinary levels of efficiency in Förster resonance energy transfer (FRET). Here, we show ultrahigh-efficiency FRET from the ensemble thin films of CdSe/CdS nanoplatelets (NPLs) to a MoS₂ monolayer. From time-resolved fluorescence spectroscopy, we observed the suppression of the photoluminescence of the NPLs corresponding to the total rate of energy transfer from ∼0.4 to 268 ns^-1. Using an Al₂O₃ separating layer between CdSe/CdS and MoS₂ with thickness tuned from 5 to 1 nm, we found that FRET takes place 7- to 88-fold faster than the Auger recombination in CdSe-based NPLs. Our measurements reveal that the FRET rate scales down with d^-2 for the donor of CdSe/CdS NPLs and the acceptor of the MoS₂ monolayer, d being the center-to-center distance between this FRET pair. A full electromagnetic model explains the behavior of this d^-2 system. This scaling arises from the delocalization of the dipole fields in the ensemble thin film of the NPLs and full distribution of the electric field across the layer of MoS₂. This d^-2 dependency results in an extraordinarily long Förster radius of ∼33 nm.