Lighting Up Yb‐MOF Across Visible and NIR Regions Through High‐Pressure Engineering

ABSTRACT Lanthanide metal‐organic frameworks (Ln‐MOFs) provide a robust platform for developing multifunctional materials with efficient dual emissions from both organic and Ln 3+ centers. However, the structural parameters that govern their intrinsic emission properties, as well as the mechanisms underlying energy transfer processes, remain poorly understood. Herein, high pressure is employed to dynamically “light up” a representative Yb‐MOF, Yb(BTC)(H 2 O) (H 3 BTC: tricarboxylate 1,3,5‐benzenetricarboxylic acid), leading to a significant emission enhancement across visible and near‐infrared regions. Pressure‐induced lattice contraction, coupled with reduced molecular vibrations and a distorted coordination environment, suppresses nonradiative losses in the organic linkers while simultaneously promoting ligand‐to‐metal energy transfer. Notably, the structural variations are retained even after decompression, resulting in a persistent, intense white‐light emission upon pressure release. This work not only elucidates the key structural factors that govern emissions in Ln‐MOFs but also demonstrates pressure engineering as a new strategy to optimize and stabilize their luminescent properties.