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

Zirkelbach J, Mirzaei M, Deperasińska I, Kozankiewicz B, Gurlek B, Shkarin A, Utikal T, Götzinger S, Sandoghdar V (2022)

Publication Type: Journal article

Publication year: 2022

Journal

Journal of Chemical Physics AIP Publishing

Book Volume: 156

Article Number: 104301

Journal Issue: 10

DOI: 10.1063/5.0081297

Abstract

Vibrational levels of the electronic ground states in dye molecules have not been previously explored at a high resolution in solid matrices. We present new spectroscopic measurements on single polycyclic aromatic molecules of dibenzoterrylene 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 to assess individual vibrational linewidths in the electronic ground state at a resolution of ∼30 MHz dictated by the linewidth of the electronic excited state. In this fashion, we identify several exceptionally narrow vibronic levels with linewidths down to values around 2 GHz. Additionally, we sample the distribution of vibronic wavenumbers, relaxation rates, and Franck-Condon factors, in both 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 density functional theory calculations. 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 create long-lived vibrational states for applications in quantum technology.

Authors with CRIS profile

Stephan Götzinger
Vahid Sandoghdar

Involved external institutions

Max-Planck-Institut für die Physik des Lichts (MPL) / Max Planck Institute for the Science of Light DE Germany (DE) Institute of Physics (IFPAN) / Instytut Fizyki PAN PL Poland (PL)

How to cite

APA:

Zirkelbach, J., Mirzaei, M., Deperasińska, I., Kozankiewicz, B., Gurlek, B., Shkarin, A.,... Sandoghdar, V. (2022). High-resolution vibronic spectroscopy of a single molecule embedded in a crystal. Journal of Chemical Physics, 156(10). https://doi.org/10.1063/5.0081297

MLA:

Zirkelbach, Johannes, et al. "High-resolution vibronic spectroscopy of a single molecule embedded in a crystal." Journal of Chemical Physics 156.10 (2022).

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