Title: Generalized Energy Gap Law: an open system dynamics approach to non-adiabatic phenomena in molecules
When: Monday, September 30, 2024, 12:00
Place: Department of Theoretical Condensed Matter Physics, Faculty of Sciences, Module 5, Seminar Room (5th Floor)
Speaker: Claudiu Genes, Head of “Quantum Cooperative Phenomena” Max-Planck-Institut für die Physik des Lichts Staudtstraße 2, 91058 Erlangen, Germany.
Non-adiabatic molecular phenomena, arising from the breakdown of the Born-Oppenheimer approximation, govern the fate of virtually all photo-physical and photo-chemical 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 [1]. We revisit and extend this theory to account for crucial aspects such as vibrational relaxation, dephasing, and radiative loss in the behavior of non-radiative processes such as, for example, internal conversion. 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 [2]. This work establishes a connection between molecular quantum optics, open quantum system dynamics and non-adiabatic molecular physics.
References
- R. Englman and J. Jortner, “The energy gap law for radiationless transitions in large molecules,” Mol. Phys. 18, 145–164 (1970)
- N. S. Baßler, M. Reitz, R. Holzinger, A. Vibok, G. J. Halasz, B. Gurlek, and C. Genes, “Generalized energy gap law: An open system dynamics approach to non-adiabatic phenomena in molecules”, arXiv:2405.08718v1 (2024)
