Tunable Circularly Polarized Luminescence by Confining Dye Molecules within Chiral Layered Metal–Organic Framework

Abstract Circularly polarized luminescence (CPL) active materials have attracted widespread attention because of their potential applications. Nonetheless, it is still a great challenge to fabricate CPL materials with both high fluorescence quantum efficiency (Φ) and high luminescent asymmetry factor (g lum ). According to the unique structure characteristics of chiral layered metal–organic frameworks (CLMOFs), herein a novel strategy to construct high‐performance CPL materials, by utilizing the confinement effect of CLMOFs is developed. Conjugate dye molecules, such as fluorescent brighteners, fluorescein, and rhodamine B, which are readily subjected to aggregation‐caused quenching (ACQ) effect, are successfully intercalated into CLMOF matrix, affording blue, yellow–green, and red CPL, respectively. Both high Φ and g lum values of up to 91% and 0.069 are obtained, owing to the distinct confinement effect of CLMOFs. After confining dye molecules within CLMOF, the ACQ effect is effectively inhibited, which is beneficial for fluorescence enhancement; simultaneously, the chirality transfer from CLMOF matrix to dyes by controlling their arrangement in the chiral confinement microenvironment, leading to the high g lum values. Based on the full‐color and strong CPL, a multi‐dimensional code system is proposed. This work paves a new avenue to design and assemble CPL materials with high Φ and g lum , which can be widely adopted.