Optical vortex generation from molecular chromophore arrays.

The generation of light endowed with orbital angular momentum, frequently termed optical vortex light, is commonly achieved by passing a conventional beam through suitably constructed optical elements. This Letter shows that the necessary phase structure for vortex propagation can be directly produced through the creation of twisted light from the vacuum. The mechanism is based on optical emission from a family of chromophore nanoarrays that satisfy specific geometric and symmetry constraints. Each such array can support pairs of electronically delocalized doubly degenerate excitons whose azimuthal phase progression is responsible for the helical wave front of the emitted radiation. The exciton symmetry dictates the maximum magnitude of topological charge; detailed analysis secures the conditions necessary to deliver optical vortices of arbitrary order.