Homochiral Metal–Organic Framework Microcrystals for Circularly Polarized Lasing

ABSTRACT Chiral framework materials offer a promising platform for exploring circularly polarized lasing. However, the creation of chirality in current optical gain framework materials relies on the chirality transfer, which suffers from weak chiral light‐matter interactions and thus limits the dissymmetry factors of circularly polarized laser emission. Here, we propose to synthesize homochiral metal–organic frameworks (MOF) from chiral optical gain molecules to enhance chiral light‐matter interactions, enabling circularly polarized lasing with large dissymmetry factors. The MOFs are grown controllably into 1D microcrystals to function as Fabry–Pérot cavities providing optical feedback for laser oscillations. In addition, the chiral optical gain molecules in the frameworks exhibit high luminescence efficiencies of ∼88% because the rigid frameworks effectively suppress nonradiative decay, resulting in low‐threshold lasing. More importantly, the homochiral optical gain frameworks can enhance chiral light‐matter interactions, which allows for circularly polarized laser emission with dissymmetry factors larger than 1.0. Our work establishes a homochiral framework material platform for exploring high‐performance circularly polarized lasing.