Creating Chiral Plasmonic Nanostructures Using Chiral Light in a Solution and on a Substrate: The Near‐Field and Hot‐Electron Routes

Abstract Can chiral light induce chiral shapes in nanocrystals in a diluted solution? So far, it has been unclear whether it could be and, if such, under which conditions it may occur. By using realistic models of plasmonic nanocrystals, this work shows that the imprinting of 3D chirality on nanocrystals in solution by circularly polarized light (CPL) is possible. Such 3D‐chiral patterns originate from the electromagnetic retardation effect. This work investigates the formation of chiral spatial distributions of the near fields and hot electrons produced by CPL in both substrate and solution settings. Anisotropic nanocrystals with sharp edges and tips are preferable for inducing 2D and 3D chirality because of the formation of chiral hot‐spot patterns on them. The 2D g‐factors are always much higher than the 3D ones. In addition, 3D‐chiral imprinting on spherical nanocrystals is impossible. With linearly polarized light (LPL), one can create chiral nanocrystals on a substrate, not in a solution. This study provides the principles for emerging technologies to create chiral nanostructures using CPL and LPL illuminations.