Distinguishing Intrinsic and Extrinsic Chirality via Dynamic Polarizability Tensor Retrieval for Maximum Optical Activity

In the landscape of plasmonic chirality, research endeavors exploring intrinsic and extrinsic chirality have progressed along distinct trajectories. However, a noteworthy observation arises from structures possessing intrinsic chirality, which exhibit extrinsic responses under tilted illumination. In this work, we establish a comprehensive connection between the polarizability tensor of metamolecules and the polarizability derived from periodic molecular wave function. Through a detailed exploration, we quantitatively and qualitatively elucidate the differences and relationships in intrinsic and extrinsic chirality generations, thereby definitively clarifying the origin of extrinsic chirality. Utilizing the superposition of extrinsic and intrinsic chirality, we also experimentally achieve the maximal optical activity of chiral metamolecules. This work advances our comprehension of optical chirality and also facilitates the design of future chiral metamolecules and their multidisciplinary applications.