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Optical Ramsey Spectroscopy on a Single Organic Molecule

Yijun Wang, Vladislav Bushmakin, Guilherme Stein, Andreas Wolfgang Schell, Ilja Gerhardt

Published Jan 1, 2023• 0 citations
Publisher

Abstract

We implement optical Ramsey spectroscopy to investigate the properties of single molecule coherence under cryogenic conditions. Our Ramsey method allows for research on a single molecule even under frequency-detuned conditions.
DOI
10.1364/cleo_fs.2023.fw4j.6

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Single molecules trapped in the solid state at liquid helium temperatures are promising quantum emitters for the development of quantum technologies owing to their remarkable photostability and their lifetime-limited optical coherence time of the order of 10 ns. The coherent preparation of their electronic state requires resonant excitation with a Rabi period much shorter than their optical coherence time. Sculpting the optical excitation with sharp edges and a high on–off intensity ratio (∼3 × 105) from a single-frequency laser beam, we demonstrate sub-nanosecond drive of a single dibenzanthanthrene molecule embedded in a naphthalene matrix at 3.2 K, over more than 17 Rabi periods. With pulses tailored for a half-Rabi period, the electronic excited state is prepared with fidelity as high as 0.97. Using single-molecule Ramsey spectroscopy, we prove up to 5 K that the optical coherence lifetime remains at its fundamental upper limit set by twice the excited-state lifetime, making single molecules suitable for quantum bit manipulations under standard cryogen-free cooling technologies.