Energy-Degenerate Photon-Pair Generation from Individual CsPbBr<sub>3</sub> Quantum Dots.

Zhu, Chenglian; Feld, Leon G; Boehme, Simon C; Cherniukh, Ihor; Bodnarchuk, Maryna I; Kovalenko, Maksym V; Rainò, Gabriele · Nano Lett · 2025

basic_science · Level V

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Abstract

Beyond single-photon emission, generating correlated <i>N</i>-photon bundles, e.g., a photon pair, is essential for various quantum technologies including quantum teleportation and metrology. A widely explored approach exploits the radiative biexciton cascade in individual (mainly epitaxially grown) quantum dots (QDs). Here, we investigate such a cascade in colloidal CsPbBr<sub>3</sub> QDs, a scalable and solution-processable quantum-light emitter. By matching their size-dependent biexciton binding energies to their size-independent phonon energies, we demonstrate the generation of time-correlated and energy-degenerate photon pairs in large (>15 nm) QDs. Under pulsed excitation at 4 K, we observe pronounced photon bunching, with a g<sup>(2)</sup>(0) of up to 7 in Hanbury Brown and Twiss measurements. The excitation-density-dependent bunching is quantitatively reproduced by multicolor numerical calculations, suggesting the cascade involving biexciton and phonon-mediated exciton decay as origin of the photon pair. Our findings provide new insights into energy-degenerate photon-pair generation in these highly engineerable quantum-light emitters, marking important steps toward their application in quantum-information technologies.