Doping MAPbBr$_3$ hybrid perovskites with CdSe/CdZnS quantum dots: from emissive thin-films to hybrid single-photon sources

Abstract

We report the first doping of crystalline methylammonium lead bromide (MAPbBr$_3$) perovskite thin-films with CdSe/CdZnS core/shell quantum dots (QDs), using a soft-chemistry method that preserves their high quantum yield and other remarkable fluorescence properties. Our approach produces MAPbBr$_3$ films of 100 nm thickness doped at volume ratios between 0.025 and 5% with colloidal CdSe/CdZnS QDs whose organic ligands are exchanged with halide ions to allow for close contact between the QDs and the perovskite matrix. Ensemble photoluminescence (PL) measurements demonstrate the retained emission of the QDs after incorporation into the MAPbBr$_3$ matrix. Ensemble photoluminescence excitation (PLE) spectra exhibit signatures of wavelength-dependent coupling between the CdSe/CdZnS QDs and the MAPbBr$_3$ matrix. Spatially-resolved PL experiments reveal a strong correlation between the positions of QDs and an enhancement of the PL signal of the matrix. Fluorescence lifetime imaging (FLIM)of the doped films furthermore show that the emission lifetime of MAPbBr$_3$ is slower in the vicinity of QDs, which, in combination with the increased PL signal of the matrix, suggests that QDs can act as nucleation seeds that improve the crystallinity of MAPbBr$_3$, boosting its emission quantum yield. Antibunching measurements provide clear evidence of single-photon emission from individual QDs-in-perovskite. Finally, the analysis of blinking statistics indicates an improvement of the photostability of individual QDs in perovskite as compared to bare CdSe/CdZnS QDs. At high doping levels, this work opens the route to hybrid-based LEDs. Low-doping content would lead to hybrid single-photon sources embedded in field-effect devices to serve as an alternative to solid-state QDs and help building nanophotonic devices with high-quantum-yield CdSe-based QDs.