Pressure‐Promoted Self‐Trapped Exciton Emission and White‐Light Harvesting in Lead Halide Metal–Organic Frameworks at Ambient Conditions

Abstract Lead halide metal−organic frameworks (MOFs) possess unique advantages in preparing single‐component white‐light‐emitting (WLE) materials due to their broadband emission based on self‐trapping excitons (STEs). However, in order to obtain high‐quality white light emission, challenges remain in adjusting and optimizing the color temperature and color coordinates of broadband STE emission. Herein, we have achieved tunable color emission and high‐quality white light emission with Commission International de l'Eclairage coordinates of (0.32, 0.38) and color temperature of 5777 K at ambient conditions in TMOF‐8(Cl) through pressure treatment. The irreversible lattice distortion after pressure treatment reduces the distance between [PbCl] + unit and TDC 2− unit. The enhanced hydrogen bonding interactions and electronic coupling between the Pb‐ s orbitals and ligand energy levels turn on the charge transfer (CT) channel from [PbCl] + unit to TDC 2− unit. Adjusting the degree of lattice distortion can achieve the regulation of the relative intensity of STE and CT emission, thereby obtaining tunable color emission and high‐quality white light emission. This study provides a new perspective on the modulation of broadband STE emission in MOFs materials and a new platform for the development of high‐quality single‐component WLE materials.