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| Autori principali: | , , , , |
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| Natura: | Preprint |
| Pubblicazione: |
2025
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| Soggetti: | |
| Accesso online: | https://arxiv.org/abs/2504.18071 |
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| _version_ | 1866910918738182144 |
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| author | Guo, Chunhao Riva, Gabriele Simoni, Jacopo Xu, Junqing Ping, Yuan |
| author_facet | Guo, Chunhao Riva, Gabriele Simoni, Jacopo Xu, Junqing Ping, Yuan |
| contents | Exciton-phonon interactions play a fundamental role in phonon-assisted radiative recombination and exciton dynamics in solids. In this work, we present a first-principles framework for computing phonon-assisted radiative lifetimes and exciton dynamics at finite temperatures. Starting from the solution of the Bethe-Salpeter equation, we construct an effective excitonic Hamiltonian that incorporates both exciton-photon and exciton-phonon interactions. Phonon-assisted radiative lifetimes in anisotropic media are evaluated using time-dependent second-order perturbation theory. We further analyze the temperature and phonon-mode dependence of phonon-assisted radiative lifetime and compare our results with available experimental data. We explain the nonmonotonic temperature dependence of the phonon-assisted radiative lifetime by different mechanisms at low and high-temperature regimes. Finally, we perform real-time exciton relaxation at the diagonal approximation of Lindbladian dynamics for time-resolved exciton occupation, providing insights into ultrafast thermalization and scattering pathways. Our ab-initio theory offers a detailed microscopic understanding of phonon-mediated exciton relaxation and recombination processes, and provides in-depth perspectives on phonon-assisted many-body interactions and their influence on optical properties for light-emitting and optoelectronic applications. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2504_18071 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Phonon-Assisted Radiative Lifetimes and Exciton Dynamics from First Principles Guo, Chunhao Riva, Gabriele Simoni, Jacopo Xu, Junqing Ping, Yuan Materials Science Exciton-phonon interactions play a fundamental role in phonon-assisted radiative recombination and exciton dynamics in solids. In this work, we present a first-principles framework for computing phonon-assisted radiative lifetimes and exciton dynamics at finite temperatures. Starting from the solution of the Bethe-Salpeter equation, we construct an effective excitonic Hamiltonian that incorporates both exciton-photon and exciton-phonon interactions. Phonon-assisted radiative lifetimes in anisotropic media are evaluated using time-dependent second-order perturbation theory. We further analyze the temperature and phonon-mode dependence of phonon-assisted radiative lifetime and compare our results with available experimental data. We explain the nonmonotonic temperature dependence of the phonon-assisted radiative lifetime by different mechanisms at low and high-temperature regimes. Finally, we perform real-time exciton relaxation at the diagonal approximation of Lindbladian dynamics for time-resolved exciton occupation, providing insights into ultrafast thermalization and scattering pathways. Our ab-initio theory offers a detailed microscopic understanding of phonon-mediated exciton relaxation and recombination processes, and provides in-depth perspectives on phonon-assisted many-body interactions and their influence on optical properties for light-emitting and optoelectronic applications. |
| title | Phonon-Assisted Radiative Lifetimes and Exciton Dynamics from First Principles |
| topic | Materials Science |
| url | https://arxiv.org/abs/2504.18071 |