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<p>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 ( &gt; 1 h), and pure (&gt; 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.</p>

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

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年1月23日

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  • Leon G. Feld,
  • Simon C. Boehme,
  • Sebastian Sabisch,
  • Nadav Frenkel,
  • Nuri Yazdani,
  • Viktoriia Morad,
  • Chenglian Zhu,
  • Taehee Kim,
  • Stefano Canossa,
  • Mariia Svyrydenko,
  • Rui Tao,
  • Maryna I. Bodnarchuk,
  • Gur Lubin,
  • Miri Kazes,
  • Vanessa Wood,
  • Dan Oron,
  • Gabriele Rainò,
  • Maksym V. Kovalenko

摘要

In lead halide perovskites (APbX3), 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 APbBr3 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 (106 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.