Abstract
Single dye molecules at cryogenic temperatures exhibit many spectroscopic phenomena known from the study of free atoms and are thus promising candidates for experiments in fundamental quantum optics. However, the existing techniques for their detection have either sacrificed information on the coherence of the excited state or have been inefficient. Here, we show that these problems can be addressed by focusing the excitation light near to the extinction cross-section of a molecule. Our detection scheme enables us to explore resonance fluorescence over nine orders of magnitude of excitation intensity and to separate its coherent and incoherent parts. In the strong excitation regime, we demonstrate the first direct observation of the Mollow fluorescence triplet from a single solid-state emitter. Under weak excitation, we report the detection of a single molecule with an incident power as faint as 600 aW, paving the way for studying nonlinear effects with only a few photons.
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References
Basché, T., Moerner, W. E., Orrit, M. & Talon, H. Photon antibunching in the fluorescence of a single dye molecule trapped in a solid. Phys. Rev. Lett. 69, 1514–1517 (1992).
Tamarat, P. et al. Pump-probe experiments with a single molecule: ac-stark effect and nonlinear optical response. Phys. Rev. Lett. 75, 1514–1518 (1995).
Tamarat, P. et al. Non-linear optical response of single molecules. Chem. Phys. 245, 121–132 (1999).
Moerner, W. E. & Kador, L. Optical detection and spectroscopy of single molecules in a solid. Phys. Rev. Lett. 62, 2535–2538 (1989).
Orrit, M. & Bernard, J. Single pentacene molecules detected by fluorescence excitation in a p-terphenyl crystal. Phys. Rev. Lett. 65, 2716–2719 (1990).
Plakhotnik, T. & Palm, V. Interferometric signatures of single molecules. Phys. Rev. Lett. 87, 183602 (2001).
Gerhardt, I. et al. Strong extinction of a laser beam by a single molecule. Phys. Rev. Lett. 98, 033601 (2007).
Turchette, Q. A., Hood, C. J., Lange, W., Mabuchi, H. & Kimble, H. J. Measurement of conditional phase shifts for quantum logic. Phys. Rev. Lett. 75, 4710–4713 (1995).
Hijlkema, M. et al. A single-photon server with just one atom. Nature Phys. 3, 253–255 (2007).
Press, D. et al. Photon antibunching from a single quantum-dot-microcavity system in the strong coupling regime. Phys. Rev. Lett. 98, 117402 (2007).
Loudon, R. Quantum Theory of Light (Oxford Univ. Press, Oxford, 2000).
Mansfield, S. M. & Kino, G. S. Solid immersion microscope. Appl. Phys. Lett. 57, 2615–2616 (1990).
Koyama, K., Yoshita, M., Baba, M., Suemoto, T. & Akiyama, H. High collection efficiency in fluorescence microscopy with a solid immersion lens. Appl. Phys. Lett. 75, 1667–1669 (1999).
van Enk, S. J. & Kimble, H. J. Strongly focused light beams interacting with single atoms in free space. Phys. Rev. A 63, 023809 (2001).
Gerardot, B. D. et al. Contrast in transmission spectroscopy of a single quantum dot. Appl. Phys. Lett. 90, 221106 (2007).
Vamivakas, A. N. et al. Strong extinction of a far-field laser beam by a single quantum dot. Nano Lett. 7, 2892–2896 (2007).
Karrai, K. & Warburton, R. J. Optical transmission and reflection spectroscopy of single quantum dots. Superlattices Microstruct. 33, 311–337 (2003).
Gerhardt, I. et al. Scanning near-field optical coherent spectroscopy of single molecules at 1.4 kelvin. Opt. Lett. 32, 1420–1422 (2007).
Cohen-Tannoudji, C., Dupont-Roc, J. & Grynberg, G. Atom-Photon Interactions (Wiley, New York, 1992).
Novotny, L., Grober, R. D. & Karrai, K. Reflected image of a strongly focused spot. Opt. Lett. 26, 789–791 (2001).
Höffges, J. T., Baldauf, H. W., Lange, W. & Walther, H. Heterodyne measurement of the resonance fluorescence of a single ion. J. Mod. Opt. 44, 1999–2010 (1997).
Mollow, B. R. Power spectrum of light scattered by two-level systems. Phys. Rev. 188, 1969–1975 (1969).
Wu, F. Y., Grove, R. E. & Ezekiel, S. Investigation of the spectrum of resonance fluorescence induced by a monochromatic field. Phys. Rev. Lett. 35, 1426–1429 (1975).
Walther, H. Advances in Atomic, Molecular and Optical Physics Vol. 51, 239–272 (Elsevier, Academic, Boston, 2005).
Hanbury Brown, R. & Twiss, R. Q. Correlation between photons in two coherent beams of light. Nature 177, 27–29 (1956).
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).
Domokos, P., Horak, P. & Ritsch, H. Quantum description of light-pulse scattering on a single atom in waveguides. Phys. Rev. A 65, 033832 (2002).
Pfab, R. J. et al. Aligned terrylene molecules in a spin-coated ultrathin crystalline film of p-terphenyl. Chem. Phys. Lett. 387, 490–495 (2004).
Dorn, R., Quabis, S. & Leuchs, G. Sharper focus for a radially polarized light beam. Phys. Rev. Lett. 91, 233901 (2003).
van Enk, S. J. Atoms, dipole waves, and strongly focused light beams. Phys. Rev. A 69, 043813 (2004).
Alù, A. & Engheta, N. Enhanced directivity from sub-wavelength infrared/optical nano-antennas loaded with plasmonic materials or metamaterials. IEEE Trans. Antennas Propagation 55, 3027–3039 (2007).
Xu, X. et al. Coherent optical spectroscopy of a strongly driven quantum dot. Science 317, 929–932 (2007).
Muller, A. et al. Resonance fluorescence from a coherently driven semiconductor quantum dot in a cavity. Phys. Rev. Lett. 99, 187402 (2007).
Boiron, A.-M., Lounis, B. & Orrit, M. Single molecules of dibenzanthanthrene in n-hexadecane. J. Chem. Phys. 105, 3969–3974 (1996).
Felekyan, S. et al. Full correlation from picoseconds to second by time-resolved and time-correlated single photon detection. Rev. Sci. Inst. 76, 083104 (2005).
Fleury, L., Segura, J.-M., Zumofen, G., Hecht, B. & Wild, U. P. Nonclassical photon statistics in single-molecule fluorescence at room temperature. Phys. Rev. Lett. 84, 1148–1151 (2000).
Lettow, R. et al. Realization of two Fourier-limited solid-state single-photon sources. Opt. Express 15, 15842–15847 (2007).
Acknowledgements
We are grateful to A. Renn for experimental support. This work was financed by the Schweizerische Nationalfond and the ETH Zurich initiative for Quantum Systems for Information Technology (QSIT).
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Wrigge, G., Gerhardt, I., Hwang, J. et al. Efficient coupling of photons to a single molecule and the observation of its resonance fluorescence. Nature Phys 4, 60–66 (2008). https://doi.org/10.1038/nphys812
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DOI: https://doi.org/10.1038/nphys812
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