Quantum beats of exciton-polarons in CsPbI3 perovskite nanocrystals
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| Main Authors: | , , , , , , , , , , , , |
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| Format: | Preprint |
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2025
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| author | Trifonov, A. V. Nestoklon, M. O. Hollberg, M. -A. Grisard, S. Kudlacik, D. Kolobkova, E. V. Kuznetsova, M. S. Goupalov, S. V. Kaspari, J. M. Reiter, D. E. Yakovlev, D. R. Bayer, M. Akimov, I. A. |
| author_facet | Trifonov, A. V. Nestoklon, M. O. Hollberg, M. -A. Grisard, S. Kudlacik, D. Kolobkova, E. V. Kuznetsova, M. S. Goupalov, S. V. Kaspari, J. M. Reiter, D. E. Yakovlev, D. R. Bayer, M. Akimov, I. A. |
| contents | Exciton-phonon interactions govern the energy level spectrum and thus the optical response in semiconductors. In this respect, lead-halide perovskite nanocrystals represent a unique system, for which the interaction with optical phonons is particularly strong, giving rise to a ladder of multiple exciton states which can be optically excited with femtosecond pulses. We establish a new regime of coherent exciton-polaron dynamics with exceptionally long coherence times (T2 ~300 ps) in an ensemble of CsPbI3 nanocrystals embedded in a glass matrix. Using transient two-pulse photon echo at 2 K temperature, we observe quantum beats between the exciton-polaron states. Within a four-level model, we directly quantify the exciton-phonon coupling strength through the Huang-Rhys factors of 0.05-0.1 and 0.02-0.04 for low-energy optical phonons with energies of 3.2 and 5.1 meV, respectively. The pronounced size dependence of both coupling strengths and phonon lifetimes offers a path to tune the optical transitions between polaron states and to tailor the coherent optical dynamics in perovskite semiconductors for solid-state quantum technologies. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2510_14695 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Quantum beats of exciton-polarons in CsPbI3 perovskite nanocrystals Trifonov, A. V. Nestoklon, M. O. Hollberg, M. -A. Grisard, S. Kudlacik, D. Kolobkova, E. V. Kuznetsova, M. S. Goupalov, S. V. Kaspari, J. M. Reiter, D. E. Yakovlev, D. R. Bayer, M. Akimov, I. A. Mesoscale and Nanoscale Physics Exciton-phonon interactions govern the energy level spectrum and thus the optical response in semiconductors. In this respect, lead-halide perovskite nanocrystals represent a unique system, for which the interaction with optical phonons is particularly strong, giving rise to a ladder of multiple exciton states which can be optically excited with femtosecond pulses. We establish a new regime of coherent exciton-polaron dynamics with exceptionally long coherence times (T2 ~300 ps) in an ensemble of CsPbI3 nanocrystals embedded in a glass matrix. Using transient two-pulse photon echo at 2 K temperature, we observe quantum beats between the exciton-polaron states. Within a four-level model, we directly quantify the exciton-phonon coupling strength through the Huang-Rhys factors of 0.05-0.1 and 0.02-0.04 for low-energy optical phonons with energies of 3.2 and 5.1 meV, respectively. The pronounced size dependence of both coupling strengths and phonon lifetimes offers a path to tune the optical transitions between polaron states and to tailor the coherent optical dynamics in perovskite semiconductors for solid-state quantum technologies. |
| title | Quantum beats of exciton-polarons in CsPbI3 perovskite nanocrystals |
| topic | Mesoscale and Nanoscale Physics |
| url | https://arxiv.org/abs/2510.14695 |