Optical Ramsey spectroscopy on a single molecule

authored by: Yijun Wang, Vladislav Bushmakin, Guilherme Alexander Stein, Andreas W. Schell, Ilja Gerhardt
Abstract: Organic chemistry offers the potential to synthesize individual molecules for specific tasks in quantum information processing. One of their striking properties is the emission of single photons with nearly ideal coherence. Here, we implement Ramsey spectroscopy to measure the electronic state coherence of a single molecule. Conventionally, the emitter’s coherence is characterized by saturation or intensity auto-correlation measurements. However, both methods are under the steady influence of continuous interaction with the excitation laser. This influence can be eliminated by using a pump–probe sequence of two optical pulses to observe the decoherence. We have measured a near-transform-limited decoherence time of 17.6 ns, while the radiative lifetime is 10.1 ns. We also perform frequency-detuned excitation, gaining richer insights into the dephasing behavior of the molecule. The experiments exhibit that optical Ramsey spectroscopy is a promising tool for measuring the emitter’s coherence properties.
Organisation(s): Surfaces Science Section
Institute of Solid State Physics
QuantumFrontiers
External Organisation(s): University of Stuttgart
Max Planck Institute for Solid State Research (MPI-FKF)
National Metrology Institute of Germany (PTB)
Type: Article
Journal: OPTICA
Volume: 9
Pages: 374-378
No. of pages: 5
ISSN: 2334-2536
Publication date: 28.03.2022
Publication status: Published
Peer reviewed: Yes
ASJC Scopus subject areas: Electronic, Optical and Magnetic Materials, Atomic and Molecular Physics, and Optics
Electronic version(s): https://doi.org/10.1364/OPTICA.443727 (Access: Open)

BibTeX

@article{8f075bfdfa4d464fb5a2365b7576c28d,
title = "Optical Ramsey spectroscopy on a single molecule",
abstract = "Organic chemistry offers the potential to synthesize individual molecules for specific tasks in quantum information processing. One of their striking properties is the emission of single photons with nearly ideal coherence. Here, we implement Ramsey spectroscopy to measure the electronic state coherence of a single molecule. Conventionally, the emitter{\textquoteright}s coherence is characterized by saturation or intensity auto-correlation measurements. However, both methods are under the steady influence of continuous interaction with the excitation laser. This influence can be eliminated by using a pump–probe sequence of two optical pulses to observe the decoherence. We have measured a near-transform-limited decoherence time of 17.6 ns, while the radiative lifetime is 10.1 ns. We also perform frequency-detuned excitation, gaining richer insights into the dephasing behavior of the molecule. The experiments exhibit that optical Ramsey spectroscopy is a promising tool for measuring the emitter{\textquoteright}s coherence properties.",
keywords = "Atomic spectroscopy, Chemistry, Electric fields, Fluorescence spectroscopy, Oscillator strengths, Quantum information processing",
author = "Yijun Wang and Vladislav Bushmakin and Stein, {Guilherme Alexander} and Schell, {Andreas W.} and Ilja Gerhardt",
note = "Funding Information: Acknowledgment. We acknowledge discussions with Dr. J. Becker, Oxford. We thank Dr. J{\"o}rg Wrachtrup for his continuous support. Funding was provided by the German Federal Ministry of Education and Research, funding program quantum technologies - from basic research to market [13N15972]. Further funding sources: Deutsche Forschungsgemeinschaft; Germany{\textquoteright}s Excellence Strategy; the COST Action “Nanoscale Quantum Optics” funded by COST.",
year = "2022",
month = mar,
day = "28",
doi = "10.1364/OPTICA.443727",
language = "English",
volume = "9",
pages = "374--378",
journal = "OPTICA",
issn = "2334-2536",
publisher = "OSA Publishing",
number = "4",
}