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Q: Fachverband Quantenoptik und Photonik

Q 46: Nano-Optics I

Q 46.3: Talk

Thursday, March 17, 2022, 11:15–11:30, Q-H11

High-resolution vibronic spectroscopy of a single molecule embedded in a crystal — •Johannes Zirkelbach1,2, Masoud Mirzaei1,2, Burak Gurlek1,2, Irena Deperasińska3, Boleslaw Kozankiewicz3, Alexey Shkarin1, Tobias Utikal1, Stephan Götzinger1,2,4, and Vahid Sandoghdar1,21Max Planck Institute for the Science of Light, 91058 Erlangen, Germany — 2Department of Physics, Friedrich-Alexander University Erlangen-Nürnberg, 91058 Erlangen, Germany — 3Institute of Physics, Polish Academy of Sciences, Al. Lotników 32/46, 02-668 Warsaw, Poland — 4Graduate School in Advanced Optical Technologies (SAOT), Friedrich Alexander University Erlangen-Nuremberg, 91052 Erlangen, Germany

Vibrational states of single organic dye molecules in solid-state hosts are known to relax within 10 ps although they could last by up to seconds in some molecules in vacuum. The resolution of conventional grating spectrometers puts a lower bound on the observed linewidths of vibrational transitions, i.e., an upper limit on measured lifetimes. Here, we present high-resolution vibronic spectra of single dibenzoterrylene molecules in para-dichlorobenzene crystals at T < 100 mK. The spectra were recorded in electronic ground and excited states using stimulated emission depletion (STED) and fluorescence excitation spectroscopy, respectively. We identified several narrow lines associated with vibrational lifetimes up to 80 ps. Using DFT calculations, we explain the intensity distribution of the vibronic lines of the dopant molecules in the solid-state environment.

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