Ultrafast non-adiabatic molecular energy conversion into photons induced by quantized electromagnetic fields

• URL: http://arxiv.org/abs/2509.13233v1
• Date: Tue, 16 Sep 2025 16:41:07 GMT
• Title: Ultrafast non-adiabatic molecular energy conversion into photons induced by quantized electromagnetic fields
• Authors: Arley Flórez López, Johan F. Triana, José Luis Sanz-Vicario,
• Abstract summary: We study the ultrafast photodynamics of diatomic molecules in confined electromagnetic fields within quantized cavities.<n>Non-adiabatic couplings play a crucial role in converting vibronic energy into photons through excited dressed states.<n>Our work paves the way for the development of many-photon generation powered by strong light-matter interaction.
• Score: 0.0
• License: http://creativecommons.org/licenses/by-nc-nd/4.0/
• Abstract: 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.

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