Bonn 2025 – wissenschaftliches Programm

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SYPE: Symposium Polaritonic Effects in Molecular Systems

SYPE 1: Polaritonic Effects in Molecular Systems

SYPE 1.3: Hauptvortrag

Dienstag, 11. März 2025, 12:00–12:30, HS 1+2

Open system dynamics for non-radiative transitions in molecules — •Claudiu Genes — TU Darmstadt, Darmstadt, and Max Planck Institute, Erlangen,Germany

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, radiative loss and most importantly, by considering higher order of non-adiabatic couplings beyond the constant case. We find closed analytical solutions allowing to decipher the mechanisms leading to non-radiative transitions. Our work establishes a connection between nanoscale quantum optics, open quantum system dynamics and non-adiabatic molecular physics and proposes an analytical approach to these processes.

Keywords: non-adiabatic; non-radiative; open system dynamics