Developing universal stimuli-responsive materials capable of emitting a broad spectrum of colors is highly desirable. Herein, we deliberately grafted a conformation-adaptable organic chromophore into the established coordination space of a flexible metal-organic framework (MOF). In terms of the coupled structural transformations and the space confinement, the chromophore in the MOF matrix underwent well-regulated conformational changes under physical and chemical stimuli, simultaneously displaying thermo-, piezo-, and solvato-fluoro-chromism with color tunability over the visible range. Owing to the resilient nature and the reduced dimensionality of the selected coordination space, all three color modulations behaved in a sensitive and self-reversible manner, each following a linear correlation of the emission maximum with stimulus. Single-crystal X-ray diffraction of the variable-temperature structures and solvent-inclusion crystals elucidated the intricate color varying mechanisms.
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http://dx.doi.org/10.1002/anie.202202073 | DOI Listing |
J Am Chem Soc
January 2025
Department of Chemistry, University of Florida, Gainesville, Florida 32611, United States.
Precisely controlling quantum states is relevant in next-generation quantum computing, encryption, and sensing. Chiral organic chromophores host unique light-matter interactions, which allow them to manipulate the quantized circular polarization of photons. Axially chiral organic scaffolds, such as helicenes or twisted acenes, are powerful motifs in chiral light manipulation.
View Article and Find Full Text PDFNat Commun
January 2025
State Key Laboratory of Superhard Materials, Synergetic Extreme Condition High-Pressure Science Center, College of Physics, Jilin University, Changchun, China.
Metal-organic frameworks that feature hybrid fluorescence and phosphorescence offer unique advantages in white-emitting communities based on their multiple emission centers and high exciton utilization. However, it poses a substantial challenge to realize superior white-light emission in single-component metal-organic frameworks without encapsulating varying chromophores or integrating multiple phosphor subunits. Here, we achieve a high-performance white-light emission with photoluminescence quantum yield of 81.
View Article and Find Full Text PDFAdv Sci (Weinh)
January 2025
Jihua Hengye Electronic Materials Co. Ltd., Foshan, Guangdong, 528200, P. R. China.
B- and N-heterocyclic fluorophores have reveal promising efficiency in blue organic light-emitting diodes (OLEDs) with small full-width-at-half-maximum (FWHM). However, their structural determinants for spectral broadening and operating stability are still needed to be investigated in further. Herein, a novel multi-N-heterocycles Diindolo[3,2,1jk:3',2',1'jk]dicarbazole[1,2-b:4,5-b] (DIDCz) is proposed to manipulate the emission color toward pure blue region by extending π-conjugation of the N-π-N bridge.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Sun Yat-Sen University, School of Chemistry, CHINA.
Immobilizing organic chromophores within the rigid framework of metal-organic frameworks (MOFs) augments fluorescence by effectively curtailing molecular motions. Yet, the substantial interspaces and free volumes inherent to MOFs can undermine photoluminescence efficiency, as they partially constrain intramolecular dynamics. In this study, we achieved optimization of both one- and two-photon excited fluorescence by incorporating linkers into an interpenetrated tetraphenylethene-based MOF (TPE-MOF).
View Article and Find Full Text PDFInorg Chem
January 2025
Department of Chemistry, University of British Columbia, Vancouver, British Columbia V6T 1Z1, Canada.
Pendant organic chromophores have been used to improve the photocatalytic performance of many metal-based photosensitizers, particularly in first-row metals, by increasing π conjugation in ligands and lowering the energy of the photoactive absorption band. Using a combination of spectroscopic studies and computational modeling, we rationalize the excited state dynamics of a Co(III) complex containing pendant pyrene moieties, , where = 1,1'-(4-(pyren-1-yl)pyridine-2,6-diyl)bis(3-methyl-1-imidazol-3-ium). displays higher visible absorptivity, and blue luminescence from pyrene singlet excited states compared with [ = 1,1'-(pyridine-2,6-diyl)bis(3-methyl-1-imidazol-3-ium)] in which the pyrene moiety is absent.
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