Photoluminescence Line Shapes of Nanocrystals: Contributions from First- and Second-Order Vibronic Couplings
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arXiv
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| Autores principales: | , , , , , |
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| Formato: | Preprint |
| Publicado: |
2026
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| _version_ | 1866917298984452096 |
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| author | Peng, Kaiyue Hou, Bokang Lin, Kailai Chen, Caroline Utzat, Hendrik Rabani, Eran |
| author_facet | Peng, Kaiyue Hou, Bokang Lin, Kailai Chen, Caroline Utzat, Hendrik Rabani, Eran |
| contents | We present a microscopic, parameter-free approach for computing the photoluminescence spectra of a single semiconductor nanocrystal. The method derives exciton-phonon coupling directly from the semi-empirical pseudopotential framework and systematically incorporates both diagonal and off-diagonal interactions, expanded to second-order in the phonon modes. The dipole-dipole correlation function was calculated using a Dyson expansion within the Kubo-Toyozawa formalism, enabling a consistent description of the role of pure dephasing and population-transfer on the photoluminescence spectral features. Applied to CdSe/CdS core-shell nanocrystals, the approach quantitatively reproduces experimental photoluminescence spectra over a wide temperature range, revealing that quadratic phonon couplings account for nearly half of the homogeneous linewidth above 100-150 K, while off-diagonal couplings leading to exciton thermalization play only a minor role and only as T approaches 300K. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2602_23604 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Photoluminescence Line Shapes of Nanocrystals: Contributions from First- and Second-Order Vibronic Couplings Peng, Kaiyue Hou, Bokang Lin, Kailai Chen, Caroline Utzat, Hendrik Rabani, Eran Chemical Physics Mesoscale and Nanoscale Physics Materials Science We present a microscopic, parameter-free approach for computing the photoluminescence spectra of a single semiconductor nanocrystal. The method derives exciton-phonon coupling directly from the semi-empirical pseudopotential framework and systematically incorporates both diagonal and off-diagonal interactions, expanded to second-order in the phonon modes. The dipole-dipole correlation function was calculated using a Dyson expansion within the Kubo-Toyozawa formalism, enabling a consistent description of the role of pure dephasing and population-transfer on the photoluminescence spectral features. Applied to CdSe/CdS core-shell nanocrystals, the approach quantitatively reproduces experimental photoluminescence spectra over a wide temperature range, revealing that quadratic phonon couplings account for nearly half of the homogeneous linewidth above 100-150 K, while off-diagonal couplings leading to exciton thermalization play only a minor role and only as T approaches 300K. |
| title | Photoluminescence Line Shapes of Nanocrystals: Contributions from First- and Second-Order Vibronic Couplings |
| topic | Chemical Physics Mesoscale and Nanoscale Physics Materials Science |
| url | https://arxiv.org/abs/2602.23604 |