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Micro-Refractometry and Local-Field Mapping with Single Molecules
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DOI：10.1021/acs.nanolett.8b01753.png)
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The refractive index n is one of the most important materials parameters of solids and, in recent years, has become the subject of significant interdisciplinary interest, especially in nanostructures and meta-materials. It is, in principle, a macroscopic quantity, so its meaning on a length scale of a few nanometers, i.e., well below the wavelength of light, is not clear a priori and is related to methods of its measurement on this length scale. Here we introduce a novel experimental approach for mapping the effective local value (n) over tilde of the refractive index in solid films and the analysis of related local-field enhancement effects. The approach is based on the imaging and spectroscopy of single chromophore molecules at cryogenic temperatures. Since the fluorescence lifetime T-1 of dye molecules in a transparent matrix depends on the refractive index due to the local density of the electromagnetic field (i.e., of the photon states), one can obtain the local (n) over tilde values in the surroundings of individual chromophores simply by measuring their T-1 times. Spatial mapping of the local (n) over tilde values is accomplished by localizing the corresponding chromophores with nanometer accuracy. We demonstrate this approach for a polycrystalline n-hexadecane film doped with terrylene. Unexpectedly large fluctuations of local-field effects and effective (n) over tilde values (the latter between 1.1 and 1.9) were found.
Keyword:
Refractive index
single-molecule spectroscopy
low temperature
zero-phonon line
point-spread function
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9.1
论文数:
2.7W
被引数:
16.5W
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