Abstract
An electronic transition between two molecular energy levels is a redistribution of electron density over the molecule’s structure following the interaction with the local electromagnetic field. Molecules that have a preferred direction for such a redistribution show a classical dipole behavior and this direction defines the excitation or emission transition dipole moment. Almost all organic dye molecules behave as electric dipole oscillators. In this chapter, we introduce two well-known methods, one for imaging the excitation transition probability, and the other for the emission transition probability of singlSSe emitters. Both of these methods are used for determining the complete three dimensional orientations of these two vectors in space. We apply them for the study of the excitation and emission properties of Carbon Nanodots (CNDs) that are novel fluorescent probes gaining popularity in bioimaging. We show that the CNDs are single dipole emitters similar to organic dyes. Thereafter, we present the first experimental method for determining the geometry of the two transition dipoles and their three-dimensional orientations simultaneously for each individual emitter. This directly gives us the angle \(\gamma \) in between both the vectors. We perform experiments on two dye molecule species, and the results show a non-negligible \(\gamma \). We speculate that this arises due to a significant rearrangement in the backbone structure of the molecule following the excitation as a result of vibrational relaxations before the emission occurs. The feasibility of these two methods for smMIET experiments is also discussed.
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Notes
- 1.
An azimuthally polarized laser has an electric field pointing in the tangential direction at each point across its cross section. When focused through an objective it has only a transverse component in the focal plane with no electric field along the optical axis.
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Karedla, N. (2017). Single-Molecule Transition Dipole Imaging. In: Single-Molecule Metal-Induced Energy Transfer. Springer Theses. Springer, Cham. https://doi.org/10.1007/978-3-319-60537-1_4
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