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.
References
Dicke, R. H. Coherence in spontaneous radiation processes. Phys. Rev. 93, 99–110 (1954).
Reitz, M., Sommer, C. & Genes, C. Cooperative quantum phenomena in light–matter platforms. PRX Quantum 3, 010201 (2022).
Lidar, D. A., Chuang, I. L. & Whaley, K. B. Decoherence-free subspaces for quantum computation. Phys. Rev. Lett. 81, 2594–2597 (1998).
Facchinetti, G., Jenkins, S. D. & Ruostekoski, J. Storing light with subradiant correlations in arrays of atoms. Phys. Rev. Lett. 117, 243601 (2016).
Beige, A., Braun, D. & Knight, P. L. Driving atoms into decoherence-free states. New J. Phys. 2, 22 (2000).
Perczel, J. et al. Topological quantum optics in two-dimensional atomic arrays. Phys. Rev. Lett. 119, 023603 (2017).
Parmee, C. D. & Ruostekoski, J. Signatures of optical phase transitions in superradiant and subradiant atomic arrays. Commun. Phys. 3, 205 (2020).
Porras, D. & Cirac, J. I. Collective generation of quantum states of light by entangled atoms. Phys. Rev. A 78, 053816 (2008).
González-Tudela, A., Paulisch, V., Chang, D. E., Kimble, H. J. & Cirac, J. I. Deterministic generation of arbitrary photonic states assisted by dissipation. Phys. Rev. Lett. 115, 163603 (2015).
Holzinger, R., Plankensteiner, D., Ostermann, L. & Ritsch, H. Nanoscale coherent light source. Phys. Rev. Lett. 124, 253603 (2020).
Berchera, I. R. & Degiovanni, I. P. Quantum imaging with sub-Poissonian light: challenges and perspectives in optical metrology. Metrologia 56, 024001 (2019).
Bettles, R. J., Gardiner, S. A. & Adams, C. S. Enhanced optical cross section via collective coupling of atomic dipoles in a 2D array. Phys. Rev. Lett. 116, 103602 (2016).
Asenjo-Garcia, A., Moreno-Cardoner, M., Albrecht, A., Kimble, H. J. & Chang, D. E. Exponential improvement in photon storage fidelities using subradiance and ‘selective radiance’ in atomic arrays. Phys. Rev. X 7, 031024 (2017).
Rui, J. et al. A subradiant optical mirror formed by a single structured atomic layer. Nature 583, 369–374 (2020).
Bekenstein, R. et al. Quantum metasurfaces with atom arrays. Nat. Phys. 16, 676–681 (2020).
Eschner, J., Raab, C., Schmidt-Kaler, F. & Blatt, R. Light interference from single atoms and their mirror images. Nature 413, 495–498 (2001).
Goban, A. et al. Superradiance for atoms trapped along a photonic crystal waveguide. Phys. Rev. Lett. 115, 063601 (2015).
McGuyer, B. H. et al. Precise study of asymptotic physics with subradiant ultracold molecules. Nat. Phys. 11, 32–36 (2015).
Solano, P., Barberis-Blostein, P., Fatemi, F. K., Orozco, L. A. & Rolston, S. L. Super-radiance reveals infinite-range dipole interactions through a nanofiber. Nat. Commun. 8, 1857 (2017).
Ferioli, G. et al. Laser-driven superradiant ensembles of two-level atoms near Dicke regime. Phys. Rev. Lett. 127, 243602 (2021).
Scheibner, M. et al. Superradiance of quantum dots. Nat. Phys. 3, 106–110 (2007).
Sipahigil, A. et al. An integrated diamond nanophotonics platform for quantum-optical networks. Science 354, 847–850 (2016).
Blach, D. D. et al. Superradiance and exciton delocalization in perovskite quantum dot superlattices. Nano Lett. 22, 7811–7818 (2022).
Hettich, C. et al. Nanometer resolution and coherent optical dipole coupling of two individual molecules. Science 298, 385–389 (2002).
Lim, S.-H., Bjorklund, T. G., Spano, F. C. & Bardeen, C. J. Exciton delocalization and superradiance in tetracene thin films and nanoaggregates. Phys. Rev. Lett. 92, 107402 (2004).
Tiranov, A. et al. Collective super- and subradiant dynamics between distant optical quantum emitters. Science 379, 389–393 (2023).
Trebbia, J.-B., Deplano, Q., Tamarat, P. & Lounis, B. Tailoring the superradiant and subradiant nature of two coherently coupled quantum emitters. Nat. Commun. 13, 2962 (2022).
Tamarat, P., Maali, A., Lounis, B. & Orrit, M. Ten years of single-molecule spectroscopy. J. Phys. Chem. A 104, 1–16 (2000).
Toninelli, C. et al. Single organic molecules for photonic quantum technologies. Nat. Mater. 20, 1615–1628 (2021).
Clear, C. et al. Phonon-induced optical dephasing in single organic molecules. Phys. Rev. Lett. 124, 153602 (2020).
Wang, D. et al. Turning a molecule into a coherent two-level quantum system. Nat. Phys. 15, 483–489 (2019).
Colautti, M. et al. Laser-induced frequency tuning of Fourier-limited single-molecule emitters. ACS Nano 14, 13584–13592 (2020).
Pazzagli, S. et al. Self-assembled nanocrystals of polycyclic aromatic hydrocarbons show photostable single-photon emission. ACS Nano 12, 4295–4303 (2018).
Nicolet, A. A. L. et al. Single dibenzoterrylene molecules in an anthracene crystal: main insertion sites. Chem. Phys. Chem. 8, 1929–1936 (2007).
Rezai, M., Wrachtrup, J. & Gerhardt, I. Coherence properties of molecular single photons for quantum networks. Phys. Rev. X 8, 031026 (2018).
Duquennoy, R. et al. Singular spectrum analysis of two-photon interference from distinct quantum emitters. Phys. Rev. Res. 5, 023191 (2023).
Wrigge, G., Gerhardt, I., Hwang, J., Zumofen, G. & Sandoghdar, V. Efficient coupling of photons to a single molecule and the observation of its resonance fluorescence. Nat. Phys. 4, 60–66 (2008).
Ambrose, W. P., Basché, T. & Moerner, W. E. Detection and spectroscopy of single pentacene molecules in a p-terphenyl crystal by means of fluorescence excitation. J. Chem. Phys. 95, 7150–7163 (1991).
Rattenbacher, D. et al. Coherent coupling of single molecules to on-chip ring resonators. New J. Phys. 21, 062002 (2019).
Paulisch, V., Perarnau-Llobet, M., González-Tudela, A. & Cirac, J. I. Quantum metrology with one-dimensional superradiant photonic states. Phys. Rev. A 99, 043807 (2019).
Tziperman, O. et al. Spontaneous emission from correlated emitters. Preprint at https://doi.org/10.48550/arXiv.2306.11348 (2023).
Gurlek, B., Sandoghdar, V. & Martin-Cano, D. Engineering long-lived vibrational states for an organic molecule. Phys. Rev. Lett. 127, 123603 (2021).
Zirkelbach, J. et al. High-resolution vibronic spectroscopy of a single molecule embedded in a crystal. J. Chem. Phys. 156, 104301 (2022).
Schädler, K. G. et al. Electrical control of lifetime-limited quantum emitters using 2D materials. Nano Lett. 19, 3789–3795 (2019).
Moradi, A., Ristanović, Z., Orrit, M., Deperasińska, I. & Kozankiewicz, B. Matrix-induced linear Stark effect of single dibenzoterrylene molecules in 2,3-dibromonaphthalene crystal. Chem. Phys. Chem 20, 55–61 (2019).
Grandi, S. et al. Quantum dynamics of a driven two-level molecule with variable dephasing. Phys. Rev. A 94, 063839 (2016).
Martín-Cano, D., Haakh, H. R., Murr, K. & Agio, M. Large suppression of quantum fluctuations of light from a single emitter by an optical nanostructure. Phys. Rev. Lett. 113, 263605 (2014).
Vivas-Viaña, A., Martín-Cano, D. & Muñoz, C. S. Dissipative stabilization of maximal entanglement between non-identical emitters via two-photon excitation. Preprint at https://arxiv.org/abs/2306.06028 (2023).
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. 20, 836–842 (2024). https://doi.org/10.1038/s41567-024-02404-4
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DOI: https://doi.org/10.1038/s41567-024-02404-4
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