Achieving Spectrally Tunable and Strong Circularly Polarized Luminescence in Zero‐Dimensional Hybrid Indium‐Antimony Halides via Dual‐Site‐Doping Strategy

Chiral zero-dimensional hybrid metal halides (0D HMHs) are notable in circularly polarized luminescence (CPL)-active materials for their chiroptical properties, yet efficient and adjustable CPL in chiral 0D HMHs remain rarely reported. This study presents a novel dual-doping strategy at A and B sites for tunable CPL in chiral 0D HMHs. For indium-based HMHs using the purely chiral cation S-2-methylpiperazine, B-site Sb³⁺ doping yields significant CPL and intense yellow fluorescence, with near-unity photoluminescence quantum yield (PLQY) and high luminescence dissymmetry factor (g_lum) of 6.7 ×1 0^-2. Notably, the introduction of 2,6-dimethylpiperazine at the A-site, alongside Sb³⁺ B-site doping, enables synergistic emission that spans blue and yellow light, thereby achieving white light emission in chiral 0D HMHs for the first time. This system achieves a PLQY of 46.08% and a g_lum of 2.1 × 10^-2, underscoring its remarkable CPL performance and spectral tunability. Near-ultraviolet pumped white light shows 25.5% polarization. This study offers a new strategy for crafting chiral 0D HMHs with tunable spectra, high PLQY, and elevated g_lum.