Surface functionalized spherical nanoparticles: an optical assessment of local chirality

Electromagnetic radiation propagating through any molecular system typically experiences a characteristic change in its polarization state as a result of light-matter interaction. Circularly polarized light is commonly absorbed or scattered to an extent that is sensitive to the incident circularity, when it traverses a medium whose constituents are chiral. This research assesses specific modifications to the properties of circularly polarized light that arise on passage through a system of surface-functionalized spherical nanoparticles, through the influence of chiral molecules on their surfaces. Non-functionalized nanospheres of atomic constitution are usually inherently achiral, but can exhibit local chirality associated with such surface-bound chromophores. The principal result of this investigation is the quantification of functionally conferred nanoparticle chirality, manifest through optical measurements such as circularly polarized emission. The relative position of chiral chromophores fixed to a nanoparticle sphere are first determined by means of spherical coverage co-ordinate analysis. The total electromagnetic field received by a spatially fixed, remote detector is then determined. It is shown that bound chromophores will accommodate both electric and magnetic dipole transition moments, whose scalar product represents the physical and mathematical origin of chiral properties identified in the detected signal. The analysis concludes with discussion of the magnitude of circular differential optical effects, and their potential significance for the characterization of surface-functionalized nanoparticles

Point source generation of chiral fields:measures of near- and far-field optical helicity

To consider the relationship between different measures of chirality in an optical field, the simplest case is considered: direct spontaneous emission of circularly polarized light by a point source. In the electromagnetic fields radiated from a suitably chiral source, such as a low-symmetry chiral molecule undergoing radiative decay, optical helicity is exhibited in the extent of a difference in left- and right-handed circular polarization components. There are several practical measures for quantifying the emergence of ensuing optical helicity, exhibiting different forms of dependence on the properties of the emitter and the positioning of a detector. By casting each measure in terms of an irreducible helicity density, connections and distinctions can be drawn between results expressible in either classical or quantum form