Harmonic spin–orbit angular momentum cascade in nonlinear optical crystals

Optical angular momentum-based photonic technologies demonstrate the key role of the optical spin–orbit interaction that usually refers to linear optical processes in spatially engineered optical materials1. Re-examining the basics of nonlinear optics of homogeneous crystals under circularly polarized light2,3, we report experiments on the enrichment of the spin–orbit angular momentum spectrum of paraxial light. The demonstration is made within the framework of second-harmonic generation using a crystal with three-fold rotational symmetry. Four spin–orbit optical states for the second harmonic field are predicted from a single fundamental state owing to the interplay between linear spin–orbit coupling and nonlinear wave mixing; three of these states are experimentally verified. Besides representing a spin-controlled nonlinear route to orbital angular multiplexing4, modal vortex light sources5,6, high-dimensional parametric processes7 and multi-state optical magnetization8, our findings suggest that the fundamentals of nonlinear optics are worth revisiting through the prism of the spin–orbit interaction of ligh