Polarization‐Directed Construction of 3D Spiral Plasmonic Micropillars for Enhanced Chiral Photoluminescence

Abstract Due to the enhanced chiral light‐matter interactions along the propagation direction of circularly polarized light, 3D chiral plasmonic nanostructures have shown exceptional chiroptic response for chiral sensing and luminescence. However, the lack of proper design and fabrication strategy causes great difficulties for achromatic chiroptic response with a high g‐factor in the visible region. Here a facile generation of 3D spiral plasmonic micropillars based on laser direct writing with a spiral vector beam is introduced. These plasmonic micropillars exhibit a dissymmetric factor (g‐factor) up to 1.0 at 800 nm, which gives rise to strong chiral plasmon photoluminescence (PL) with an achromatic luminescence dissymmetry (g lum ) up to 0.4 across the visible region (500–750 nm). Furthermore, cathodoluminescence (CL) characterizations of these spiral micropillars reveal a location‐selective chiral inversion of the CL spectra, which is related to the variation of the superchiral fields within the spiral micropillars. This work not only establishes a facile, efficient and enantioselective paradigm for the optical generation of 3D chiral plasmonic nanostructures but also reveals the crucial role of superchiral field in both the chiral PL and CL, which is significant for the development of superior chiral luminescence devices.