Phonon-driven wavefunction localization promotes room-temperature, pure single-photon emission in large organic-inorganic lead-halide perovskite quantum dots
Gabriele Raino a b, Feld Leon a b, Simon C. Boehme a b, Maryna Bodnarchuk b, Nuri Yadzani c, Dan Oron d, Maksym Kovalenko a b
a Institute of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, CH-8093 Zürich, Switzerland
b Laboratory for Thin Films and Photovoltaics, Empa – Swiss Federal Laboratories for Materials Science and Technology, CH-8600 Dübendorf, Switzerland
c Department of Information Technology and Electrical Engineering, ETH Zürich, CH-8093 Zürich, Switzerland
d Department of Molecular Chemistry and Materials Science, Weizmann Institute of Science, Rehovot 76100, Israel
Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
Advances in Nanocrystals: Fundamental approaches and technological perspectives - #NCAdv
Sevilla, Spain, 2025 March 3rd - 7th
Organizers: Carmelita Rodà and Matteo Zaffalon
Invited Speaker, Gabriele Raino, presentation 103
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.103
Publication date: 16th December 2024

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-cation in soft APbBr3 colloidal quantum dots (QDs) controls the phonon-induced localization of the exciton wavefunction. Insights from ab initio molecular dynamics and single-particle fluorescence spectroscopy demonstrate that anharmonic lattice vibrations and the resulting polymorphism 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 (>1h), and pure (>95%) single-photon emission in a widely tuneable spectral range (495-745 nm). Strong electron-phonon interaction in soft perovskite QDs provides an unconventional route toward the development of scalable room-temperature quantum light sources.

 

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