Non-lorentzian single-molecule line shape: pseudolocal phonons and coherence transfer
The excitation line shape of a single terrylene molecule in a naphthalene crystal has been investigated. In addition to the conventional Lorentzian, it consists of a dispersive component in the core region and a sideband. This is due to a pseudolocal phonon caused by the substitution of a host molecule with the chromophore. When the pseudolocal phonon is excited, the resonance frequency of the chromophore slightly changes, resulting in the appearance of a second, quasiresonant transition. Coherence transfer between these two optical transitions causes the deviation from the purely Lorentzian line shape.
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Physical Chemistry Laboratory, Swiss Federal Institute of Technology, ETH-Zentrum, CH-8092 Zurich, Switzerland.
Plakhotnik
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