Ultrafast non-adiabatic molecular energy conversion into photons induced by quantized electromagnetic fields
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arXiv
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| Natura: | Preprint |
| Pubblicazione: |
2025
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| _version_ | 1866914040469520384 |
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| author | López, Arley Flórez Triana, Johan F. Sanz-Vicario, José Luis |
| author_facet | López, Arley Flórez Triana, Johan F. Sanz-Vicario, José Luis |
| contents | Molecular polaritons within the mid-infrared regime have emerged as a source for modifying and manipulating molecular and photonic properties. However, the development of new methodologies for photon generation is still a challenge in nanophotonics. We propose a molecular model based on the Holstein-quantum-Rabi Hamiltonian, which also incorporates realistic dipole moments and non-adiabatic couplings among electronic excited states, to study the ultrafast photodynamics of diatomic molecules in confined electromagnetic fields within quantized cavities. In addition to vibronic transitions due to intrinsic non-adiabatic couplings, two types of light-induced crossings emerge: one type is located at molecular nuclear geometries where the rotating wave approximation is fulfilled, and another type appears at different geometries where counter-rotating transitions may occur. We make a comprehensive study of polariton photodynamics within a time window of a few tens of femtoseconds, where dissipative mechanisms do not influence the polariton photodynamics. We stress the dramatic change of the polariton energy spectrum as a function of the Huang-Rhys factor when non-adiabatic couplings are included in the model. We conclude that both the molecular non-adiabatic couplings and, more specifically, the counter-rotating couplings in the cavity-molecule interaction play a crucial role in converting vibronic energy into photons through excited dressed states. We also show that the sign of the Huang-Rhys factor has a significant impact on this photon conversion. Our work paves the way for the development of many-photon generation powered by strong light-matter interaction, along with potential applications using alkaline earth monohydride molecules. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2509_13233 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Ultrafast non-adiabatic molecular energy conversion into photons induced by quantized electromagnetic fields López, Arley Flórez Triana, Johan F. Sanz-Vicario, José Luis Quantum Physics Molecular polaritons within the mid-infrared regime have emerged as a source for modifying and manipulating molecular and photonic properties. However, the development of new methodologies for photon generation is still a challenge in nanophotonics. We propose a molecular model based on the Holstein-quantum-Rabi Hamiltonian, which also incorporates realistic dipole moments and non-adiabatic couplings among electronic excited states, to study the ultrafast photodynamics of diatomic molecules in confined electromagnetic fields within quantized cavities. In addition to vibronic transitions due to intrinsic non-adiabatic couplings, two types of light-induced crossings emerge: one type is located at molecular nuclear geometries where the rotating wave approximation is fulfilled, and another type appears at different geometries where counter-rotating transitions may occur. We make a comprehensive study of polariton photodynamics within a time window of a few tens of femtoseconds, where dissipative mechanisms do not influence the polariton photodynamics. We stress the dramatic change of the polariton energy spectrum as a function of the Huang-Rhys factor when non-adiabatic couplings are included in the model. We conclude that both the molecular non-adiabatic couplings and, more specifically, the counter-rotating couplings in the cavity-molecule interaction play a crucial role in converting vibronic energy into photons through excited dressed states. We also show that the sign of the Huang-Rhys factor has a significant impact on this photon conversion. Our work paves the way for the development of many-photon generation powered by strong light-matter interaction, along with potential applications using alkaline earth monohydride molecules. |
| title | Ultrafast non-adiabatic molecular energy conversion into photons induced by quantized electromagnetic fields |
| topic | Quantum Physics |
| url | https://arxiv.org/abs/2509.13233 |