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Electrostatic Boundary Conditions in Dielectrics01:27

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Surface orientation ambiguity for single molecules at dielectric interfaces.

E Dey, M Elorza, F W Foss

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    Defocus fluorescence microscopy can determine molecule orientation, but surface proximity causes measurement errors. New finite-element modeling corrects these errors for accurate orientation determination near interfaces.

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    Area of Science:

    • Optical Biophysics
    • Surface Science
    • Computational Modeling

    Background:

    • Fluorescent molecules emit light in a dipole radiation pattern.
    • Defocused fluorescence microscopy infers molecular orientation from this pattern.
    • Accurate orientation measurement relies on precise mathematical modeling.

    Purpose of the Study:

    • To identify and address an ambiguity in common calculations of dipole radiation patterns.
    • To investigate the impact of dielectric surfaces on measured molecular orientation.
    • To provide a method for correcting orientation measurements for molecules near interfaces.

    Main Methods:

    • Analysis of mathematical models for dipole radiation patterns near dielectric surfaces.
    • Comparison of theoretical predictions with experimental data.
    • Application of finite-element modeling to simulate on-surface emitters between dielectric media.

    Main Results:

    • An ambiguity in standard calculations leads to erroneous dipole rotation towards dielectric surfaces.
    • This rotation can be misinterpreted as preferential horizontal molecular orientation.
    • Finite-element modeling successfully resolves the theoretical ambiguity.

    Conclusions:

    • Common orientation calculations are compromised for molecules near dielectric interfaces.
    • A new theoretical treatment considering finite current elements is required.
    • A prescription for correcting measured orientations at arbitrary interfaces is provided.