Doping MAPbBr3 hybrid perovskites with CdSe/CdZnS quantum dots: from emissive thin films to hybrid single-photon sources

Abstract

We report the first doping of crystalline methyl–ammonium lead bromide perovskite (MAPbBr₃) films with CdSe/CdZnS core/shell quantum dots (QDs), using a soft-chemistry approach that preserves their high quantum yield and other remarkable luminescence properties. Our approach produces MAPbBr₃ films of around 100 nm thickness, doped at volume ratios between 0.01 and 1% with colloidal CdSe/CdZnS QDs whose organic ligands were 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 MAPbBr₃ matrix. Photoluminescence excitation (PLE) spectra exhibit signatures of wavelength-dependent coupling between the CdSe/CdZnS QDs and the MAPbBr₃ matrix, i.e., a transfer of charges from matrix to QD, which increases the QD luminescence by up to 150%, or from QD to matrix. Spatially-resolved PL experiments reveal a strong correlation between the positions of QDs and an enhancement of the PL signal of the matrix. Lifetime imaging of the doped films furthermore shows that the emission lifetime of MAPbBr₃ is slower in the vicinity of QDs, which, in combination with the increased PL signal of the matrix, suggests that QDs can act as local nucleation seeds that improve the crystallinity of MAPbBr₃, thus boosting its emission quantum yield. Luminescence 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 CdSe/CdZnS QD doping levels, this work thus opens a route to hybrid solar concentrators for visible-light harvesting and hybrid-based LEDs, while a low degree of doping could yield hybrid single-photon sources than can be embedded in field-effect devices for single-charge control, which would allow the construction of nanophotonic devices via low-cost solution-processing techniques as an alternative to solid-state quantum dots.