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.
On-chip interference of scattering from two individual molecules
Dominik Rattenbacher,
Alexey Shkarin,
Jan Renger,
Tobias Utikal,
Stephan Götzinger,
Vahid Sandoghdar
Integrated photonic circuits offer a promising route for studying coherent cooperative effects of a controlled collection of quantum emitters. However, spectral inhomogeneities, decoherence, and material incompatibilities in the solid state make this a nontrivial task. Here, we demonstrate efficient coupling of a pair of Fourier-limited organic molecules embedded in a polyethylene film to a TiO2 microdisc resonator on a glass chip. Moreover, we tune the resonance frequencies of the emitters with respect to that of the microresonator by employing nanofabricated electrodes. For two molecules separated by a distance of about 8 µm and an optical phase difference of about pi/2, we report on a large collective extinction of the incident light in the forward direction and the destructive interference of its scattering in the backward direction. Our work sets the ground for coherent coupling of several quantum emitters via a common mode and realization of polymer-based hybrid quantum photonic circuits.
Quantum Efficiency of Single Dibenzoterrylene Molecules in p-Dichlorobenzene at Cryogenic Temperatures
Mohammad Musavinezhad,
Alexey Shkarin,
Dominik Rattenbacher,
Jan Renger,
Tobias Utikal,
Stephan Götzinger,
Vahid Sandoghdar
The Journal of Physical Chemistry B
5353-5359
(2023)
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We measure the quantum efficiency (QE) of individual dibenzoterrylene (DBT) molecules embedded in p-dichlorobenzene at cryogenic temperatures. To achieve this, we combine two distinct methods based on the maximal photon emission and on the power required to saturate the zero-phonon line to compensate for uncertainties in some key system parameters. We find that the outcomes of the two approaches are in good agreement for reasonable values of the parameters involved, reporting a large fraction of molecules with QE values above 50%, with some exceeding 70%. Furthermore, we observe no correlation between the observed lower bound on the QE and the lifetime of the molecule, suggesting that most of the molecules have a QE exceeding the established lower bound. This confirms the suitability of DBT for quantum optics experiments. In light of previous reports of low QE values at ambient conditions, our results hint at the possibility of a strong temperature dependence of the QE.
Max-Planck-Zentren und -Schulen
Datenerfassung
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