Breaking the blue limit of non-conjugated hydrocarbons via multiple through-space interactionsOA
The development of non-conjugated luminescent systems has innovated the traditional design strategy of through-bond conjugation(TBC)and inspired a deeper understanding on molecular photophysics.However,a challenge encountered by these non-conjugated structures is that the fluorescence of pure hydrocarbon systems is largely confined to the blue region(∼470 nm),raising the question of whether this is a fundamental limitation.Herein,we break this barrier by constructing a library of over 50 non-conjugated arylated alkenes via binuclear nickel-catalyzed hydroarylation of allenes.It is disclosed that synergistic multiple through-space interactions(TSIs)including molecular twisting-tuned intramolecular TSIs combined with intermolecular TSIs mediated by the double bonds of styrene units are critical for achieving the ultralong-wavelength aggregation-induced emission of these non-conjugated structures.This enables tunable light emission from blue to yellow,orange and,remarkably,even to single-compound-based warm white light.Furthermore,strategic substitution extends the fluorescence into the deep-red region,with a tail reaching 900 nm.This work demonstrates that non-conjugated pure hydrocarbons can achieve a broad spectrum of colors,fundamentally advancing the understanding of the luminescence phenomenon of non-conjugated systems and providing a novel design strategy for luminescent materials beyond the traditional TBC paradigm.
Shuxin Jiang;Ziwei Deng;Xiaoming Wang;Zheng Zhao;Ben Zhong Tang
State Key Laboratory of Organometallic Chemistry and Shanghai-Hong Kong Joint Laboratory in Chemical Synthesis,Shanghai Institute of Organic Chemistry,University of Chinese Academy of Sciences,Chinese Academy of Sciences,Shanghai 200032,ChinaGuangdong Basic Research Center of Excellence for Aggregate Science,School of Science and Engineering,Shenzhen Institute of Aggregate Science and Technology,The Chinese University of Hong Kong(Shenzhen),Shenzhen 518172,ChinaState Key Laboratory of Organometallic Chemistry and Shanghai-Hong Kong Joint Laboratory in Chemical Synthesis,Shanghai Institute of Organic Chemistry,University of Chinese Academy of Sciences,Chinese Academy of Sciences,Shanghai 200032,China School of Chemistry and Materials Science,Hangzhou Institute for Advanced Study,University of Chinese Academy of Sciences,Hangzhou 310024,China School of Chemistry and Chemical Engineering,Henan Normal University,Xinxiang 453007,ChinaGuangdong Basic Research Center of Excellence for Aggregate Science,School of Science and Engineering,Shenzhen Institute of Aggregate Science and Technology,The Chinese University of Hong Kong(Shenzhen),Shenzhen 518172,ChinaGuangdong Basic Research Center of Excellence for Aggregate Science,School of Science and Engineering,Shenzhen Institute of Aggregate Science and Technology,The Chinese University of Hong Kong(Shenzhen),Shenzhen 518172,China
通用工业技术
through-space interactionnon-conventional luminescent materialsaggregation-induced emissionhydroarylationallenes
《National Science Review》 2026 (11)
P.281-293,13
supported by the National Key R&D Program of China(2022YFA1503200 and 2023YFB3810001)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB0610000,XDB1180000)the National Natural Science Foundation of China(92256303,22171278 and 52273197)the Open Project of State Key Laboratory of Synergistic Chem-Bio Synthesis(sklscbs202503)Shanghai Municipal Science and Technology Major Project,the Shanghai Science and Technology Committee(23ZR1482400)the Natural Science Foundation of Ningbo(2023J034)financial support from Guangdong Basic Research Center of Excellence for Aggregate Science,the Science Technology Innovation Commission of Shenzhen Municipality(GJHZ20210705141810031 and KQTD20210811090142053).
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