Spin-orbit interactions and chiroptical effects engaging orbital angular momentum of twisted light in chiral and achiral media

TL;DR

This paper develops a theoretical framework to understand how spin-orbit interactions involving orbital angular momentum of twisted light influence chiroptical effects, enabling discrimination of chiral and achiral media through optical processes.

Contribution

It introduces a novel mechanism involving optical spin-orbit interactions with electric quadrupole moments, clarifying how these effects differ in chiral and achiral media.

Findings

Identifies spin-orbit interactions engaging electric quadrupole moments.

Differentiates symmetry criteria for 2D and 3D chirality.

Explains optical discrimination mechanisms in media.

Abstract

There is recurrent interest in the orbital angular momentum (OAM) conveyed by optical vortices, which are structured beams with a helically twisted wavefront. Particular significance is attached to the issue of how, in its interactions with matter, light conveying OAM might prove sensitive to the relative handedness and degree of twist in the associated optical wavefront. As a result of recent experimental and theoretical studies, the supposition that beams with OAM might enable discrimination between oppositely handed forms of matter has become a renewed focus of attention. Some of the tantalizing conclusions that are beginning to emerge from this research have, however, not yet established a definitive basis for a supporting mechanism. To resolve this problem requires the development of theory to support a faithful representation, and a thorough understanding, of the fundamental molecule-photon physics at play in such optical processes, even for processes as basic as absorption. The present analysis establishes mechanisms at play that entail a novel manifestation of optical spin-orbit interactions (SOI), engaging transition electric quadrupole moments. Moreover, powerful symmetry principles prove to render distinctively different criteria governing the exhibition of 2D and 3D chirality. The new results elucidate the operation of such effects, identifying their responsibility for discriminatory optical interactions of various forms in both chiral and achiral media.