Phonon-driven wavefunction localization enhances room-temperature single-photon purity in large hybrid lead halide perovskite quantum dots.

Feld, Leon G; Boehme, Simon C; Sabisch, Sebastian; Frenkel, Nadav; Yazdani, Nuri; Morad, Viktoriia; Zhu, Chenglian; Kim, Taehee et al. · Nat Commun · 2026

basic_science · Level V

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Abstract

In lead halide perovskites (APbX<sub>3</sub>), the effect of the A-site cation on optical and electronic properties has initially been thought to be marginal. Yet, evidence of beneficial effects on solar-cell performance and light emission is accumulating. Here, we report that the A-site cation in soft APbBr<sub>3</sub> colloidal quantum dots (QDs) controls the phonon-induced localization of the exciton wavefunction. Insights from ab-initio molecular-dynamics simulations and single-particle fluorescence spectroscopy demonstrate that anharmonic crystal vibrations and the resulting disorder act as an additional confinement potential. Avoiding the trade-off between single-photon purity and optical stability faced by downsizing conventional QDs into the strong confinement regime, dynamical phonon-induced confinement in large organic-inorganic perovskite QDs enables bright (10<sup>6</sup> photons/s), stable ( > 1 h), and pure (> 95%) single-photon emission tunable across a wide spectral range (495-745 nm). Strong electron-phonon interaction in soft perovskite QDs provides an unconventional route toward developing scalable room-temperature quantum-light sources.