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Measurement of Three-Dimensional Dipole Orientation of a Single Fluorescent Nanoemitter by Emission Polarization Analysis

Abstract : We demonstrate theoretically and experimentally that the three-dimensional orientation of a single fluorescent nanoemitter can be determined by polarization analysis of the emitted light (while excitation polarization analysis provides only the in-plane orientation). The determination of the emitter orientation by polarimetry requires a theoretical description, including the objective numerical aperture, the 1D or 2D nature of the emitting dipole, and the environment close to the dipole. We develop a model covering most experimentally relevant microscopy configurations and provide analytical relations that are useful for orientation measurements. We perform polarimetric measurements on high-quality core-shell CdSe/CdS nanocrystals and demonstrate that they can be approximated by two orthogonal degenerated dipoles. Finally, we show that the orientation of a dipole can be inferred by polarimetric measurement, even for a dipole in the vicinity of a gold film, while in this case, the well-established defocused microscopy is not appropriate.
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PhysRevX.4.021037.pdf
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Clotilde Lethiec, Julien Laverdant, Henri Vallon, Clémentine Javaux, Benoît Dubertret, et al.. Measurement of Three-Dimensional Dipole Orientation of a Single Fluorescent Nanoemitter by Emission Polarization Analysis. Physical Review X, American Physical Society, 2014, 4 (2), pp.021037. ⟨10.1103/PhysRevX.4.021037⟩. ⟨hal-01340131⟩

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