Integrating Achiral and Chiral Organic Ligands in Zero‐Dimensional Hybrid Metal Halides to Boost Circularly Polarized Luminescence

Abstract Chiral zero‐dimensional hybrid metal halides (0D HMHs) could combine excellent optical properties and chirality, making them promising for circularly polarized luminescence (CPL). However, chiral 0D HMHs with efficient CPL have been rarely reported. Here, we propose an efficient strategy to achieve simultaneously high photoluminescence quantum yield (PLQY) and large dissymmetry factor ( g lum ), by integrating achiral and chiral ligands into 0D HMHs. Specifically, three pairs of chiral 0D hybrid indium‐antimony chlorides are synthesized by combing achiral guanidine with three types of chiral methylbenzylammonium‐based derivatives as the organic cations. These chiral 0D HMHs exhibit near‐unity PLQY and large g lum values up to around ±1×10 −2 . The achiral guanidine ligand is not only essential to crystallize these hybrid indium‐antimony chlorides to achieve near‐unity PLQYs, but also greatly enhances the chirality induction from organic ligands to inorganic units in these 0D HMHs. Furthermore, the choice of different chiral ligands can modify the strength of hydrogen bonding interactions in these 0D HMHs, to maximize their g lum values. Overall, this study provides a robust way to realize efficient CPL in chiral HMHs, expanding their applications in chiroptical fields.