Abstract
Future quantum communication will rely on the integration of single-photon sources, quantum memories and systems with strong single-photon nonlinearities1. Two key parameters are crucial for the single-photon source: a high photon flux with a very small bandwidth, and a spectral match to other components of the system. Atoms or ions may act as single-photon sources—owing to their narrowband emission and their intrinsic spectral match to other atomic systems—and can serve as quantum nonlinear elements. Unfortunately, their emission rates are still limited, even for highly efficient cavity designs2. Single solid-state emitters such as single organic dye molecules are significantly brighter3 and allow for narrowband photons4; they have shown potential in a variety of quantum optical experiments5,6 but have yet to be interfaced with other components such as stationary memory qubits. Here we describe the optical interaction between Fourier-limited photons from a single organic molecule and atomic alkali vapours, which can constitute an efficient quantum memory. Single-photon emission rates reach up to several hundred thousand counts per second and show a high spectral brightness of 30,000 detectable photons per second per megahertz of bandwidth. The molecular emission is robust and we demonstrate perfect tuning to the spectral transitions of the sodium D line and efficient filtering, even for emitters at ambient conditions. In addition, we achieve storage of molecular photons originating from a single dibenzanthanthrene molecule in atomic sodium vapour. Given the large set of molecular emission lines matching to atomic transitions, our results enable the combination of almost ideal single-photon sources with various atomic vapours, such that experiments with giant single-photon nonlinearities, mediated, for example, by Rydberg atoms7,8, become feasible.
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References
Kimble, H. J. The quantum internet. Nature 453, 1023–1030 (2008)
Nisbet-Jones, P. B. R., Dilley, J., Ljunggren, D. & Kuhn, A. Highly efficient source for indistinguishable single photons of controlled shape. New J. Phys. 13, 103036 (2011)
Lee, K. et al. A planar dielectric antenna for directional single-photon emission and near-unity collection efficiency. Nature Photon. 5, 166–169 (2011)
Lounis, B. & Orrit, M. Single-photon sources. Rep. Prog. Phys. 68, 1129–1179 (2005)
Hettich, C. et al. Nanometer resolution and coherent optical dipole coupling of two individual molecules. Science 298, 385–389 (2002)
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. Nature Phys. 4, 60–66 (2008)
Dudin, Y. O. & Kuzmich, A. Strongly interacting Rydberg excitations of a cold atomic gas. Science 336, 887–889 (2012)
Firstenberg, O. et al. Attractive photons in a quantum nonlinear medium. Nature 502, 71–75 (2013)
Boiron, A.-M., Lounis, B. & Orrit, M. Single molecules of dibenzanthanthrene in n-hexadecane. J. Chem. Phys. 105, 3969–3974 (1996)
Lettow, R. et al. Realization of two Fourier-limited solid-state single-photon sources. Opt. Express 15, 15842–15847 (2007)
Petelski, T., Fattori, M., Lamporesi, G., Stuhler, J. & Tino, G. Doppler-free spectroscopy using magnetically induced dichroism of atomic vapor: a new scheme for laser frequency locking. Eur. Phys. J. D 22, 279–283 (2003)
Wild, U. P., Güttler, F., Pirotta, M. & Renn, A. Single molecule spectroscopy: Stark effect of pentacene in p-terphenyl. Chem. Phys. Lett. 193, 451–455 (1992)
Orrit, M., Bernard, J., Zumbusch, A. & Personov, R. Stark effect on single molecules in a polymer matrix. Chem. Phys. Lett. 196, 595–600 (1992)
Nicolet, A. A. L., Hofmann, C., Kol'chenko, M. A., Kozankiewicz, B. & Orrit, M. Single dibenzoterrylene molecules in an anthracene crystal: spectroscopy and photophysics. ChemPhysChem 8, 1215–1220 (2007)
Pirotta, M., Renn, A., Werts, M. H. & Wild, U. P. Single molecule spectroscopy. Perylene in the Shpol'skiĭ matrix n-nonane. Chem. Phys. Lett. 250, 576–582 (1996)
Nonn, T. & Plakhotnik, T. Fluorescence excitation spectroscopy of vibronic transitions in single molecules. Chem. Phys. Lett. 336, 97–104 (2001)
Kiraz, A., Ehrl, M., Bräuchle, C. & Zumbusch, A. Low temperature single molecule spectroscopy using vibronic excitation and dispersed fluorescence detection. J. Chem. Phys. 118, 10821–10824 (2003)
Dick, D. J. & Shay, T. M. Ultrahigh-noise rejection optical filter. Opt. Lett. 16, 867–869 (1991)
Harrell, S. D. et al. Sodium and potassium vapor Faraday filters revisited: theory and applications. J. Opt. Soc. Am. B 26, 659–670 (2009)
Akopian, N., Wang, L., Rastelli, A., Schmidt, O. G. & Zwiller, V. Hybrid semiconductor-atomic interface: slowing down single photons from a quantum dot. Nature Photon. 5, 230–233 (2011)
Tey, M. K. et al. Strong interaction between light and a single trapped atom without the need for a cavity. Nature Phys. 4, 924–927 (2008)
Pritchard, J. D. et al. Cooperative atom-light interaction in a blockaded Rydberg ensemble. Phys. Rev. Lett. 105, 193603 (2010)
Parigi, V. et al. Observation and measurement of interaction-induced dispersive optical nonlinearities in an ensemble of cold Rydberg atoms. Phys. Rev. Lett. 109, 233602 (2012)
Gerhardt, I. et al. Coherent state preparation and observation of Rabi oscillations in a single molecule. Phys. Rev. A 79, 011402 (2009)
Peloso, M. P., Gerhardt, I., Ho, C., Lamas-Linares, A. & Kurtsiefer, C. Daylight operation of a free space, entanglement-based quantum key distribution system. New J. Phys. 11, 045007 (2009)
Mais, S., Basche, T., Mueller, G., Müllen, K. & Bräuchle, C. Probing the spectral dynamics of single terrylenediimide molecules in low-temperature solids. Chem. Phys. 247, 41–52 (1999)
Kiraz, A., Ehrl, M., Bräuchle, C. & Zumbusch, A. Ultralong coherence times in the purely electronic zero-phonon line emission of single molecules. Appl. Phys. Lett. 85, 920–922 (2004)
Jelezko, F., Tamarat, P., Lounis, B. & Orrit, M. Dibenzoterrylene in naphthalene: a new crystalline system for single molecule spectroscopy in the near infrared. J. Phys. Chem. 100, 13892–13894 (1996)
Kummer, S., Basche, T. & Bräuchle, C. Terrylene in p-terphenyl: a novel single crystalline system for single molecule spectroscopy at low temperatures. Chem. Phys. Lett. 229, 309–316 (1994)
Kummer, S. et al. Absorption, excitation, and emission spectroscopy of terrylene in p-terphenyl: bulk measurements and single molecule studies. J. Chem. Phys. 107, 7673–7684 (1997)
Kitson, S. C., Jonsson, P., Rarity, J. G. & Tapster, P. R. Intensity fluctuation spectroscopy of small numbers of dye molecules in a microcavity. Phys. Rev. A 58, 620–627 (1998)
Boyd, R. W. & Gauthier, D. J. in Progress in Optics Vol. 43, Ch. 6, 497–530 (Elsevier, 2002)
Shi, Z., Boyd, R. W., Camacho, R. M., Vudyasetu, P. K. & Howell, J. C. Slow-light Fourier transform interferometer. Phys. Rev. Lett. 99, 240801 (2007)
Acknowledgements
We thank W. Kiefer for the calculation of the sodium-2-FADOF transmission (Fig. 3). G.S. acknowledges support by J. Pflaum (University of Würzburg). I.G. acknowledges discussions with R. Löw and S. Hofferberth (University of Stuttgart). J.W. acknowledges support by the Max Planck Society (via a Max Planck fellowship), the BMBF (via the projects QuORep and Q.com) and the EU (via the project SIQS and the ERC grant SQUTEC).
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Contributions
I.G. conceived the idea. P.S., G.S. and I.G. prepared and conducted the experiments. I.G. and J.W. supervised the team and wrote the manuscript.
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Extended data figures and tables
Extended Data Figure 1 Imaging fluorescent samples, supported by atomic vapour.
Single fluorescent bead, imaged in a confocal microscope, illuminated with laser light, locked to the crossover resonance of the sodium D2 transition. Although the overall count rate does not substantially differ, the signal-to-noise ratio is measured to be 210 when using the commercial filter, and 240 when only the sodium filter is used. Integration time per pixel is 2 ms.
Extended Data Figure 2 Combined spectroscopy of DBT and potassium.
Spectra of single DBT molecules and atomic K vapour on the K D2 line around 766 nm. The molecules in the sample are sparse. Therefore, the image represents multiple recordings at several lateral positions.
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Siyushev, P., Stein, G., Wrachtrup, J. et al. Molecular photons interfaced with alkali atoms. Nature 509, 66–70 (2014). https://doi.org/10.1038/nature13191
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DOI: https://doi.org/10.1038/nature13191
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