Abstract
An array of radiatively coupled emitters provides a platform for generating, storing and manipulating quantum light. However, the simultaneous positioning and tuning of several lifetime-limited emitters into resonance remains a challenge. Here we report the creation of superradiant and subradiant entangled states in pairs of lifetime-limited and subwavelength-spaced organic molecules by permanently shifting them into resonance with laser-induced tuning. The molecules are embedded as defects in an organic nanocrystal. The pump light redistributes charges in the nanocrystal and dramatically increases the likelihood of resonant molecules. The frequency spectra, lifetimes and second-order correlation functions agree with a simple quantum model. This scalable tuning approach with organic molecules provides a pathway for observing collective quantum phenomena in subwavelength arrays of quantum emitters.
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Data availability
All data supporting this study are available from figshare at https://doi.org/10.6084/m9.figshare.24969456. Source data are provided with this paper.
Code availability
The simulation code is available from figshare at https://doi.org/10.6084/m9.figshare.24969456.
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Acknowledgements
J.H. and L.H. acknowledge support from the National Science Foundation (Grant No. DMREF-2324299) and the Office of Science of the US Department of Energy through the Quantum Science Center, a National Quantum Information Science Research Center. We thank C. Toninelli and A. Clark for nanocrystal synthesis and characterization advice.
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J.H. and L.H. conceived the experiment. C.L. and J.H. designed the experiment, performed the numerical simulations and wrote the paper. C.L. and E.D. collected the data. C.L., V.W. and J.H. performed the analytic calculations. All authors interpreted the results.
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Lange, C.M., Daggett, E., Walther, V. et al. Superradiant and subradiant states in lifetime-limited organic molecules through laser-induced tuning. Nat. Phys. (2024). https://doi.org/10.1038/s41567-024-02404-4
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DOI: https://doi.org/10.1038/s41567-024-02404-4
