Chemo- and Thermomechanically Configurable 3D Optical Metamaterials Constructed from Colloidal Nanocrystal Assemblies

Nanofabrication has limited most optical metamaterials to 2D or, often with multiple patterning steps, simple 3D meta-atoms that typically have limited built-in tunability. Here, with a one-step scalable patterning process, we exploit the chemical addressability and structural adaptability of colloidal Au nanocrystal assemblies to transform 2D nanocrystal/Ti bilayers into complex, 3D-structured meta-atoms and to thermally direct their shape morphing and alter their optical properties. By tailoring the length, number, and curvature of 3D helical structures in each meta-atom, we create large-area metamaterials with chiroptical responses of as high as ∼40% transmission difference between left-hand (LCP) and right-hand (RCP) circularly polarized light (ΔT = T_RCP - T_LCP) that are suitable for broadband circular polarizers and, upon thermally configuring their shape, switch the polarity of polarization rotation. These 3D optical metamaterials provide prototypes for low-cost, large-scale fabrication of optical metamaterials for ultrathin lenses, polarizers, and waveplates.