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.