Photon statistics of scattered light and generalized birefringence experiments

Abstract

The theoretical dependence of optical birefringence phenomena on the statistical nature of the light is investigated. Photon S-matrix calculations lead to expressions relating the change induced in the statistical nature of the beam to the molecular properties of the target sample. A hypothetical generalized optical birefringence experiment is analysed: in the experiment the coincidences of photons arriving at spatially separated detectors sensitive to different polarizations are observed with and without the sample in the beam, and the difference in the photon correlations depend on the initial statistical composition and polarization of the beam and the molecular properties of the sample. When the beam is generated by a thermal source the difference of the signals (with and without the sample) depends on the product of the polarizability and optical rotation tensors. When the light is generated by a single-mode coherent source the statistical properties of the light are such as to eliminate the second-order interaction terms, and so the experiment yields the hyperpolarizability and hyper-rotation tensors automatically and with the explicit exclusion of the polarization and rotation tensor contributions.