Circularly polarized light is incident on a nanostructured chiral meta‐surface. In the nanostructured unit cells whose chirality matches that of light, superchiral light is forming and strong optical second harmonic generation can be observed.
We studied the adsorption kinetics of supported ultrathin films of dye-labeled polystyrene (l-PS) by combining dielectric spectroscopy (DS) and the interface-specific nonlinear optical second harmonic generation (SHG) technique. While DS is sensitive to the fraction of mobile dye moieties (chromophores), the SHG signal probes their anisotropic orientation. Time-resolved measurements were performed above the glass transition temperature on two different sample geometries. In one configuration, the l-PS layer is placed in contact with the aluminum surface, while in the other one, the deposition is done on a strongly adsorbed layer of neat PS. From the time dependence of the dielectric strength and SHG signal of the l-PS layer in contact with the metal, we detected two different kinetics regimes. We interpret these regimes in terms of the interplay between adsorption and orientation of the adsorbing labeling moieties. At early times, dye moieties get adsorbed adopting an orientation parallel to the surface. When adsorption proceeds to completeness, the kinetics slows down and the dye moieties progressively orient normal to the surface. Conversely, when the layer of l-PS layer is deposited on the strongly adsorbed layer of neat PS, both the dielectric strength and the SHG signal do not show any variation with time. This means that no adsorption takes place.
k Cambridge ? Buffalo Faraday rotation, the rotation of the polarization of light due to a magnetic field in the direction of propagation of the light, is used in applications ranging from quantum memory to the detection of biomagnetic fields. For these applications large Faraday rotation is necessary, but absorption of light is detrimental. In search of these properties, we have characterized the Verdet constant of a so far unexplored class of mesogenic organic molecules. We report their spectra and provide an interpretation. A Verdet constant of almost 2.5• 10 5 deg T 1 m 1 is found around 520 nm. This Verdet constant is three orders of magnitude larger than the largest known for organic molecules in a region without spectral features. We attribute this enormous Faraday rotation to resonant enhancement by a triplet excitation which does not appear in the linear absorption spectrum, and near-resonant enhancement by low-energy singlet excitations. Furthermore we are able to switch the Faraday rotation by changing the liquid crystal phase of the compound. These results demonstrate a new class of Faraday rotating materials with great potential to replace current materials and improve existing applications. The inherent flexibility in the synthesis of this class of molecules opens a new field of research in Faraday rotation.
Abstract:While it has been demonstrated that, above its resolution limit, Second Harmonic Generation (SHG) microscopy can map chiral local field enhancements, below that limit, structural defects were found to play a major role. Here we show that, even below the resolution limit, the contributions from chiral local field enhancements to the SHG signal can dominate over those by structural defects. We report highly homogeneous SHG micrographs of star-shaped gold nanostructures, where the SHG circular dichroism effect is clearly visible from virtually every single nanostructure. Most likely, size and geometry determine the dominant contributions to the SHG signal in nanostructured systems.
References and links1. J. B. Pendry, "A chiral route to negative refraction," Science 306(5700), 1353-1355 (2004 1983-1986 (1983). 7. T. Petralli-Mallow, T. M. Wong, J. D. Byers, H. I. Yee, and J. M. Hicks, "Circular dichroism spectroscopy at interfaces: a surface second harmonic generation study," J. Phys. Chem. 97(7), 1383-1388 (1993). 8. P. Fischer and F. Hache, "Nonlinear optical spectroscopy of chiral molecules," Chirality 17(8), 421-437 (2005).
Circularly polarized light imparts a sense of rotation on the electron density in ring‐shaped gold nanostructures. As a consequence, the near‐field enhancement becomes homogeneous on the surface of the nanostructures, thereby increasing the opportunity for interaction with molecules. This type of nanostructured samples can find a broad range of applications in chemical processes where the interaction between molecules and local field enhancements play an important role.
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