In our project, we explore different schemes for studying the dynamics and energetic states of molecular vibrations at temperatures down to 20 mK.
High-resolution vibronic spectroscopy of a single molecule embedded in a
crystal
Johannes Zirkelbach, Masoud Mirzaei, Irena Deperasińska, Boleslaw Kozankiewicz, Burak Gürlek, Alexey Shkarin, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar
The Journal of Chemical Physics
156
104301
(2022)
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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.
Spectral splitting of a stimulated Raman transition in a single molecule
Johannes Zirkelbach, Burak Gürlek, Masoud Mirzaei, Alexey Shkarin, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar
Physical Review Research
5
043244
(2023)
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The small cross-section of Raman scattering poses a great challenge for its direct study at the single-molecule level. By exploiting the high Franck-Condon factor of a common-mode resonance, choosing a large vibrational frequency difference in electronic ground and excited states and operating at T<2K, we succeed at driving a coherent stimulated Raman transition in individual molecules. We observe and model a spectral splitting that serves as a characteristic signature of the phenomenon at hand. Our study sets the ground for exploiting the intrinsic optomechanical degrees of freedom of molecules for applications in solid-state quantum optics and information processing.