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| Main Authors: | , , , , , , , , , , , , , , , |
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| Format: | Preprint |
| Published: |
2024
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| Subjects: | |
| Online Access: | https://arxiv.org/abs/2404.15920 |
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| _version_ | 1866917649021140992 |
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| author | Feld, Leon G. Boehme, Simon C. Sabisch, Sebastian Frenkel, Nadav Yazdani, Nuri Morad, Viktoriia Zhu, Chenglian Svyrydenko, Mariia Tao, Rui Bodnarchuk, Maryna Lubin, Gur Kazes, Miri Wood, Vanessa Oron, Dan Rainò, Gabriele Kovalenko, Maksym V. |
| author_facet | Feld, Leon G. Boehme, Simon C. Sabisch, Sebastian Frenkel, Nadav Yazdani, Nuri Morad, Viktoriia Zhu, Chenglian Svyrydenko, Mariia Tao, Rui Bodnarchuk, Maryna Lubin, Gur Kazes, Miri Wood, Vanessa Oron, Dan Rainò, Gabriele Kovalenko, Maksym V. |
| contents | 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 (10^6 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. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2404_15920 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Phonon-driven wavefunction localization promotes room-temperature, pure single-photon emission in large organic-inorganic lead-halide quantum dots Feld, Leon G. Boehme, Simon C. Sabisch, Sebastian Frenkel, Nadav Yazdani, Nuri Morad, Viktoriia Zhu, Chenglian Svyrydenko, Mariia Tao, Rui Bodnarchuk, Maryna Lubin, Gur Kazes, Miri Wood, Vanessa Oron, Dan Rainò, Gabriele Kovalenko, Maksym V. Materials Science 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 (10^6 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. |
| title | Phonon-driven wavefunction localization promotes room-temperature, pure single-photon emission in large organic-inorganic lead-halide quantum dots |
| topic | Materials Science |
| url | https://arxiv.org/abs/2404.15920 |