The dark exciton ground state promotes photon-pair emission in individual perovskite nanocrystals

• Published in: Nature communications Vol. 11; no. 1; p. 6001
• Main Authors: Tamarat, Philippe, Hou, Lei, Trebbia, Jean-Baptiste, Swarnkar, Abhishek, Biadala, Louis, Louyer, Yann, Bodnarchuk, Maryna I., Kovalenko, Maksym V., Even, Jacky, Lounis, Brahim
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group 26.11.2020; Nature Publishing Group UK; Nature Portfolio
• Subjects: Anisotropy; Cesium; Crystals; Emitters; Emitters (electron); Excitons; Fine structure; Holes (electron deficiencies); Iodides; Lead; Lead compounds; Light emission; Low temperature; Metal halides; Nanocrystals; Optical properties; Optoelectronics; Perovskites; Photoluminescence; Photons; Physics; Quantum Physics; Recombination; Thermal coupling; Ultrastructure
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-020-19740-7

Abstract Cesium lead halide perovskites exhibit outstanding optical and electronic properties for a wide range of applications in optoelectronics and for light-emitting devices. Yet, the physics of the band-edge exciton, whose recombination is at the origin of the photoluminescence, is not elucidated. Here, we unveil the exciton fine structure of individual cesium lead iodide perovskite nanocrystals and demonstrate that it is governed by the electron-hole exchange interaction and nanocrystal shape anisotropy. The lowest-energy exciton state is a long-lived dark singlet state, which promotes the creation of biexcitons at low temperatures and thus correlated photon pairs. These bright quantum emitters in the near-infrared have a photon statistics that can readily be tuned from bunching to antibunching, using magnetic or thermal coupling between dark and bright exciton sublevels.