Room-Temperature, Highly Pure Single-Photon Sources from All-Inorganic Lead Halide Perovskite Quantum Dots

Nano Lett. 2022 May 11;22(9):3751-3760. doi: 10.1021/acs.nanolett.2c00756. Epub 2022 Apr 25.

Abstract

Attaining pure single-photon emission is key for many quantum technologies, from optical quantum computing to quantum key distribution and quantum imaging. The past 20 years have seen the development of several solid-state quantum emitters, but most of them require highly sophisticated techniques (e.g., ultrahigh vacuum growth methods and cryostats for low-temperature operation). The system complexity may be significantly reduced by employing quantum emitters capable of working at room temperature. Here, we present a systematic study across ∼170 photostable single CsPbX3 (X: Br and I) colloidal quantum dots (QDs) of different sizes and compositions, unveiling that increasing quantum confinement is an effective strategy for maximizing single-photon purity due to the suppressed biexciton quantum yield. Leveraging the latter, we achieve 98% single-photon purity (g(2)(0) as low as 2%) from a cavity-free, nonresonantly excited single 6.6 nm CsPbI3 QDs, showcasing the great potential of CsPbX3 QDs as room-temperature highly pure single-photon sources for quantum technologies.

Keywords: perovskite quantum dots; photostable photoluminescence; quantum light; single quantum dot spectroscopy; single-photon purity.