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| Auteurs principaux: | , , , |
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| Format: | Preprint |
| Publié: |
2024
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| Accès en ligne: | https://arxiv.org/abs/2409.18287 |
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| _version_ | 1866915445217427456 |
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| author | Gómez-Bastidas, A. F. Sriram, Karthik Garcia-Castro, A. C. Rubel, Oleg |
| author_facet | Gómez-Bastidas, A. F. Sriram, Karthik Garcia-Castro, A. C. Rubel, Oleg |
| contents | We performed high-throughput density functional theory calculations of optical matrix elements between band edges across a diverse set of non-magnetic two-dimensional monolayers with direct band gaps. Materials were ranked as potential optical emitters, leading to the identification of transition-metal nitrogen halides (ZrNCl, TiNBr, TiNCl) and bismuth chalcohalides (BiTeCl) with optical coupling comparable to or exceeding MoS$_2$. Despite strong in-plane dipole transitions, most two-dimensional materials underperform bulk semiconductors due to the absence of out-of-plane components. To elucidate interband transitions, we introduced the orbital overlap tensor and established a correlation between anomalous Born effective charges and optical coupling, linking charge redistribution to transition strength. We also identified chalcogen-mediated $d$-$d$ transition as a key mechanism enabling optical responses in transition-metal dichalcogenides. We derived an analytical radiative recombination model incorporating multi-valley effects and found that excitonic corrections are essential for accurate lifetime predictions. Some direct-gap materials exhibit dark excitons as their lowest-energy states, classifying them as quasi-direct band gap semiconductors, which is critical for tuning excitonic recombination dynamics. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2409_18287 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Efficiency of band edge optical transitions of 2D monolayer materials: A high-throughput computational study Gómez-Bastidas, A. F. Sriram, Karthik Garcia-Castro, A. C. Rubel, Oleg Materials Science Mesoscale and Nanoscale Physics Computational Physics We performed high-throughput density functional theory calculations of optical matrix elements between band edges across a diverse set of non-magnetic two-dimensional monolayers with direct band gaps. Materials were ranked as potential optical emitters, leading to the identification of transition-metal nitrogen halides (ZrNCl, TiNBr, TiNCl) and bismuth chalcohalides (BiTeCl) with optical coupling comparable to or exceeding MoS$_2$. Despite strong in-plane dipole transitions, most two-dimensional materials underperform bulk semiconductors due to the absence of out-of-plane components. To elucidate interband transitions, we introduced the orbital overlap tensor and established a correlation between anomalous Born effective charges and optical coupling, linking charge redistribution to transition strength. We also identified chalcogen-mediated $d$-$d$ transition as a key mechanism enabling optical responses in transition-metal dichalcogenides. We derived an analytical radiative recombination model incorporating multi-valley effects and found that excitonic corrections are essential for accurate lifetime predictions. Some direct-gap materials exhibit dark excitons as their lowest-energy states, classifying them as quasi-direct band gap semiconductors, which is critical for tuning excitonic recombination dynamics. |
| title | Efficiency of band edge optical transitions of 2D monolayer materials: A high-throughput computational study |
| topic | Materials Science Mesoscale and Nanoscale Physics Computational Physics |
| url | https://arxiv.org/abs/2409.18287 |