Metasurfaces and Colloidal Suspensions Composed of 3D Chiral Si Nanoresonators

High‐refractive‐index silicon nanoresonators are promising low‐loss alternatives to plasmonic particles in CMOS‐compatible nanophotonics applications. However, complex 3D particle morphologies are challenging to realize in practice, thus limiting the range of achievable optical functionalities. Using 3D film structuring and a novel gradient mask transfer technique, the first intrinsically chiral dielectric metasurface is fabricated in the form of a monolayer of twisted silicon nanocrescents that can be easily detached and dissolved into colloidal suspension. The metasurfaces exhibit selective handedness and a circular dichroism as large as 160° µm^?1 due to pronounced differences in induced current loops for left‐handed and right‐handed polarization. The detailed morphology of the detached particles is analyzed using high‐resolution transmission electron microscopy. Furthermore, it is shown that the particles can be manipulated in solution using optical tweezers. The fabrication and detachment method can be extended to different nanoparticle geometries and paves the way for a wide range of novel nanophotonic experiments and applications of high‐index dielectrics.