Single-photon superradiance in individual caesium lead halide quantum dots

• 成果类型: Article
• 署名作者: Zhu, Chenglian; Boehme, Simon C.; Feld, Leon G.; Moskalenko, Anastasiia; Dirin, Dmitry N.; Mahrt, Rainer F.; Stoeferle, Thilo; Bodnarchuk, Maryna I.; Efros, Alexander L.; Sercel, Peter C.; Kovalenko, Maksym V.; Raino, Gabriele
• 署名单位: Swiss Federal Institutes of Technology Domain; ETH Zurich; Swiss Federal Institutes of Technology Domain; Swiss Federal Laboratories for Materials Science & Technology (EMPA); United States Department of Defense; United States Navy
• 刊物名称: Nature
• ISSN/ISSBN: 0028-5299
• DOI: 10.1038/s41586-023-07001-8
• 发表日期: 2024-02-15
• 页码: 535-+
• 关键词: perovskite nanocrystals; radiative decay; emission; excitons; pseudopotentials; nanoplatelets; absorption; cspbx3; br

摘要

The brightness of an emitter is ultimately described by Fermi's golden rule, with a radiative rate proportional to its oscillator strength times the local density of photonic states. As the oscillator strength is an intrinsic material property, the quest for ever brighter emission has relied on the local density of photonic states engineering, using dielectric or plasmonic resonators(1,2). By contrast, a much less explored avenue is to boost the oscillator strength, and hence the emission rate, using a collective behaviour termed superradiance. Recently, it was proposed(3) that the latter can be realized using the giant oscillator-strength transitions of a weakly confined exciton in a quantum well when its coherent motion extends over many unit cells. Here we demonstrate single-photon superradiance in perovskite quantum dots with a sub-100 picosecond radiative decay time, almost as short as the reported exciton coherence time(4). The characteristic dependence of radiative rates on the size, composition and temperature of the quantum dot suggests the formation of giant transition dipoles, as confirmed by effective-mass calculations. The results aid in the development of ultrabright, coherent quantum light sources and attest that quantum effects, for example, single-photon emission, persist in nanoparticles ten times larger than the exciton Bohr radius.