Generalized energy gap law: An open system dynamics approach to non-adiabatic phenomena in molecules

• URL: http://arxiv.org/abs/2405.08718v1
• Date: Tue, 14 May 2024 15:59:58 GMT
• Title: Generalized energy gap law: An open system dynamics approach to non-adiabatic phenomena in molecules
• Authors: N. S. Bassler, M. Reitz, R. Holzinger, A. Vibók, G. J. Halász, B. Gurlek, C. Genes,
• Abstract summary: Non-adiabatic molecular phenomena govern the fate of virtually all photo-physical and photochemical processes. A simple and elegant description, the energy gap law, was derived five decades ago. We revisit and extend this theory to account for crucial aspects such as vibrational relaxation, dephasing, and radiative loss.
• Score: 0.0
• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: Non-adiabatic molecular phenomena, arising from the breakdown of the Born-Oppenheimer approximation, govern the fate of virtually all photo-physical and photochemical processes and limit the quantum efficiency of molecules and other solid-state embedded quantum emitters. A simple and elegant description, the energy gap law, was derived five decades ago, predicting that the non-adiabatic coupling between the excited and ground potential landscapes lead to non-radiative decay with a quasi-exponential dependence on the energy gap. We revisit and extend this theory to account for crucial aspects such as vibrational relaxation, dephasing, and radiative loss. We find a closed analytical solution with general validity which indicates a direct proportionality of the non-radiative rate with the vibrational relaxation rate at low temperatures, and with the dephasing rate of the electronic transition at high temperatures. Our work establishes a connection between nanoscale quantum optics, open quantum system dynamics and non-adiabatic molecular physics.

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