The role of dark polariton states for electronic strong coupling in molecules
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arXiv
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| Format: | Preprint |
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2025
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| _version_ | 1866918106267385856 |
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| author | Borges, Lucas Schnappinger, Thomas Kowalewski, Markus |
| author_facet | Borges, Lucas Schnappinger, Thomas Kowalewski, Markus |
| contents | Polaritonic chemistry investigates the possible modification of chemical and photochemical reactions by means of strong light-matter coupling in optical cavities, as demonstrated in numerous experiments over the last few years. These experiments are typically interpreted in terms of the Jaynes-Cummings or Tavis-Cummings models under the assumption that the molecular ensemble is only excited by a single photon. In such a model, two polariton states compete with an overwhelming number of dark states, inhibiting polaritonic reactions entropically. We analyze the higher excitation manifolds of the Tavis-Cummings model along with a three-level system that resembles photochemical reactions. We demonstrate that allowing for more than a single excitation makes the reaction of the involved polaritons entropically more favorable. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2504_20798 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | The role of dark polariton states for electronic strong coupling in molecules Borges, Lucas Schnappinger, Thomas Kowalewski, Markus Quantum Physics Chemical Physics Polaritonic chemistry investigates the possible modification of chemical and photochemical reactions by means of strong light-matter coupling in optical cavities, as demonstrated in numerous experiments over the last few years. These experiments are typically interpreted in terms of the Jaynes-Cummings or Tavis-Cummings models under the assumption that the molecular ensemble is only excited by a single photon. In such a model, two polariton states compete with an overwhelming number of dark states, inhibiting polaritonic reactions entropically. We analyze the higher excitation manifolds of the Tavis-Cummings model along with a three-level system that resembles photochemical reactions. We demonstrate that allowing for more than a single excitation makes the reaction of the involved polaritons entropically more favorable. |
| title | The role of dark polariton states for electronic strong coupling in molecules |
| topic | Quantum Physics Chemical Physics |
| url | https://arxiv.org/abs/2504.20798 |