Fischer, Eric Wolfgang
[Verfasser:in]
;
Saalfrank, Peter
[Akademische:r Betreuer:in];
Vendrell, Oriol
[Akademische:r Betreuer:in];
Kühn, Oliver
[Akademische:r Betreuer:in]Universität Potsdam
Quantum vibrational dynamics in complex environments: from vibrational strong coupling in molecular cavity QED to phonon-induced adsorbate relaxation
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Hochschulschrift
Titel:
Quantum vibrational dynamics in complex environments: from vibrational strong coupling in molecular cavity QED to phonon-induced adsorbate relaxation
Hochschulschrift:
Dissertation, Universität Potsdam, 2022
Anmerkungen:
Beschreibung:
Molecules are often naturally embedded in a complex environment. As a consequence, characteristic properties of a molecular subsystem can be substantially altered or new properties emerge due to interactions between molecular and environmental degrees of freedom. The present thesis is concerned with the numerical study of quantum dynamical and stationary properties of molecular vibrational systems embedded in selected complex environments. In the first part, we discuss "strong-coupling" model scenarios for molecular vibrations interacting with few quantized electromagnetic field modes of an optical Fabry-Pérot cavity. We thoroughly elaborate on properties of emerging "vibrational polariton" light-matter hybrid states and examine the relevance of the dipole self-energy. Further, we identify cavity-induced quantum effects and an emergent dynamical resonance in a cavity-altered thermal isomerization model, which lead to significant suppression of thermal reaction rates. [...]