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High-resolution vibronic spectroscopy of a single molecule embedded in a crystal

MPS-Authors
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Zirkelbach,  Johannes
Sandoghdar Division, Max Planck Institute for the Science of Light, Max Planck Society;

/persons/resource/persons270607

Mirzaei,  Masoud
Sandoghdar Division, Max Planck Institute for the Science of Light, Max Planck Society;

/persons/resource/persons220989

Gürlek,  Burak
Sandoghdar Division, Max Planck Institute for the Science of Light, Max Planck Society;

/persons/resource/persons228904

Shkarin,  Alexey
Sandoghdar Division, Max Planck Institute for the Science of Light, Max Planck Society;

/persons/resource/persons201220

Utikal,  Tobias
Sandoghdar Division, Max Planck Institute for the Science of Light, Max Planck Society;

/persons/resource/persons201072

Götzinger,  Stephan
Sandoghdar Division, Max Planck Institute for the Science of Light, Max Planck Society;

/persons/resource/persons201175

Sandoghdar,  Vahid
Sandoghdar Division, Max Planck Institute for the Science of Light, Max Planck Society;

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Citation

Zirkelbach, J., Mirzaei, M., Deperasińska, I., Kozankiewicz, B., Gürlek, B., Shkarin, A., et al. (2022). High-resolution vibronic spectroscopy of a single molecule embedded in a crystal. The Journal of Chemical Physics, 156: 104301. doi:10.1063/5.0081297.


Cite as: https://hdl.handle.net/21.11116/0000-0009-9EB6-8
Abstract
Vibrational levels of the electronic ground states in dye molecules have not been previously explored at high resolution
in solid matrices. We present new spectroscopic measurements on single polycyclic aromatic molecules of dibenzoter-
rylene embedded in an organic crystal made of para-dichlorobenzene. To do this, we use narrow-band continuous-wave
lasers and combine spectroscopy methods based on fluorescence excitation and stimulated emission depletion (STED)
to select individual vibronic transitions at a resolution of ∼30 MHz dictated by the linewidth of the electronic ex-
cited state. In this fashion, we identify several exceptionally narrow vibronic levels in the electronic ground state with
linewidths down to values around 2 GHz. Additionally, we sample the distribution of vibronic wavenumbers, relax-
ation rates, and Franck-Condon factors, both in the electronic ground and excited states for a handful of individual
molecules. We discuss various noteworthy experimental findings and compare them with the outcome of DFT cal-
culations. The highly detailed vibronic spectra obtained in our work pave the way for studying the nanoscopic local
environment of single molecules. The approach also provides an improved understanding of the vibrational relaxation
mechanisms in the electronic ground state, which may help to create long-lived vibrational states for applications in
quantum technology.