Guest Entrapment in Metal‐Organic Nanosheets for Quantifiably Tuneable Luminescence

Abstract Luminescent metal‐organic frameworks (LMOFs) are promising materials for nanophotonic applications due to their tuneable structure and programmability. Yet, the 3D nature of LMOFs creates challenges for stability, optical transparency, and device integration. Metal‐organic nanosheets (MONs) potentially overcome these limitations by combining the benefits of metal‐organic frameworks (MOFs) with an atomically thin morphology of large planar dimensions. Herein, the bottom‐up synthesis of few‐layer thin ZIF‐7‐III MONs via facile low‐energy salt‐templating is reported. Employing guest@MOF design, the fluorophores Rhodamine B and Fluorescein are intercalated into ZIF‐7 nanosheets (Z7‐NS) to form light emissive systems exhibiting intense and highly photostable fluorescence. Aggregation and Förster resonance energy transfer, enabled by the MON framework, are revealed as the mechanisms behind fluorescence. By varying guest concentration, these mechanisms provide predictable quantified control over emission chromaticity of a dual‐guest Z7‐NS material and the definition of an “emission chromaticity fingerprint” – a unique subset of the visible spectrum that a material can emit by fluorescence.