Excitonic Mott transition without population inversion
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arXiv
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| Autores principales: | , , , , , , , , , , , , , , |
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| Formato: | Preprint |
| Publicado: |
2026
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| _version_ | 1866910112533184512 |
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| author | Dogadov, Oleg Genco, Armando Cadore, Allison R. Kerfoot, James A. Alexeev, Evgeny M. Balci, Osman Trovatello, Chiara Watanabe, Kenji Taniguchi, Takashi Tongay, Seth Ariel Ferrari, Andrea C. Cerullo, Giulio Conte, Stefano Dal Stefanucci, Gianluca Perfetto, Enrico |
| author_facet | Dogadov, Oleg Genco, Armando Cadore, Allison R. Kerfoot, James A. Alexeev, Evgeny M. Balci, Osman Trovatello, Chiara Watanabe, Kenji Taniguchi, Takashi Tongay, Seth Ariel Ferrari, Andrea C. Cerullo, Giulio Conte, Stefano Dal Stefanucci, Gianluca Perfetto, Enrico |
| contents | Exciton dissociation via the excitonic Mott transition (EMT) governs the high-density optical response of semiconductors and sets fundamental limits for optoelectronic devices. The EMT is conventionally linked to the onset of population inversion and the emergence of optical gain. Here, we demonstrate that this paradigm can break down under ultrafast non-equilibrium excitation. Using femtosecond pump-probe optical spectroscopy, we drive a monolayer transition metal dichalcogenide into a dense photoexcited state in which the excitonic resonance is completely quenched within ~100 fs, while the optical gain is entirely absent across the explored fluence range. State-of-the-art real-time ab initio simulations reveal that the EMT is governed by an interplay of strongly nonthermal carrier populations and nonequilibrium dynamical screening of the Coulomb interaction. The quantitative agreement between theory and experiment identifies a distinct, ultrafast pathway to exciton ionization beyond quasi-equilibrium descriptions and demonstrates that population inversion is not a universal prerequisite for the EMT. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2604_06897 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Excitonic Mott transition without population inversion Dogadov, Oleg Genco, Armando Cadore, Allison R. Kerfoot, James A. Alexeev, Evgeny M. Balci, Osman Trovatello, Chiara Watanabe, Kenji Taniguchi, Takashi Tongay, Seth Ariel Ferrari, Andrea C. Cerullo, Giulio Conte, Stefano Dal Stefanucci, Gianluca Perfetto, Enrico Mesoscale and Nanoscale Physics Exciton dissociation via the excitonic Mott transition (EMT) governs the high-density optical response of semiconductors and sets fundamental limits for optoelectronic devices. The EMT is conventionally linked to the onset of population inversion and the emergence of optical gain. Here, we demonstrate that this paradigm can break down under ultrafast non-equilibrium excitation. Using femtosecond pump-probe optical spectroscopy, we drive a monolayer transition metal dichalcogenide into a dense photoexcited state in which the excitonic resonance is completely quenched within ~100 fs, while the optical gain is entirely absent across the explored fluence range. State-of-the-art real-time ab initio simulations reveal that the EMT is governed by an interplay of strongly nonthermal carrier populations and nonequilibrium dynamical screening of the Coulomb interaction. The quantitative agreement between theory and experiment identifies a distinct, ultrafast pathway to exciton ionization beyond quasi-equilibrium descriptions and demonstrates that population inversion is not a universal prerequisite for the EMT. |
| title | Excitonic Mott transition without population inversion |
| topic | Mesoscale and Nanoscale Physics |
| url | https://arxiv.org/abs/2604.06897 |