Harvesting Multicolor Photoluminescence in Nonaromatic Interpenetrated Metal–Organic Framework Nanocrystals via Pressure‐Modulated Carbonyls Aggregation

Abstract Interpenetrated metal–organic frameworks (MOFs) with nonaromatic ligands provide a unique platform for adsorption, catalysis, and sensing applications. However, nonemission and the lack of optical property tailoring make it challenging to fabricate smart responsive devices with nonaromatic interpenetrated MOFs based on ligand‐centered emission. In this paper, the pressure‐induced aggregation effect is introduced in nonaromatic interpenetrated Zn 4 O(ADC) 4 (Et 3 N) 6 (IRMOF‐0) nanocrystals (NCs), where carbonyl groups aggregation results in O ─ O distances smaller than the sum of the van der Waals radii (3.04 Å), triggering the photoluminescence turn‐on behavior. It is noteworthy that the IRMOF‐0 NCs display an ultrabroad emission tunability of 130 nm from deep blue (440 nm) to yellow (570 nm) upon release to ambient conditions at different pressures. The eventual retention of through‐space n–π* interactions in different degrees via pressure treatment is primarily responsible for achieving a controllable multicolor emission behavior in initially nonemissive IRMOF‐0 NCs. The fabricated multicolor phosphor‐converted light‐emitting diodes based on the pressure‐treated IRMOF‐0 NCs exhibit excellent thermal, chromaticity, and fatigue stability. The proposed strategy not only imparts new vitality to nonaromatic interpenetrated MOFs but also offers new perspectives for advancements in the field of multicolor displays and daylight illumination.