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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Preorganized helical chirality controlled homochiral self-assembly and circularly polarized luminescence of a quadruple-stranded Eu2L4 helicate
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Preorganized helical chirality controlled homochiral self-assembly and circularly polarized luminescence of a quadruple-stranded Eu2L4 helicate

机译：预染色螺旋手性控制的冠编自组装和圆形绞合EU2L4螺旋的圆偏振发光

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摘要

beta-Diketones are one of the most widely used ligands for sensitizing the luminescence of lanthanide complexes due to their excellent sensitization abilities. However, the difficulties in introducing chiral groups to take part in the electronic transitions of conjugated systems limit their application in lanthanide circularly polarized luminescence (CPL) materials. In view of the inherent chirality of the helical structure, herein, a pair of homochiral quadruple-stranded helicates, Eu2L4, is assembled based on chiral bis-beta-diketonate ligands, wherein the two point chirality centers in the spacer preorganize the helical conformation of the ligand (3S,4S)/(3R,4R)-3,4-bis(4,4'-bis(4,4,4-trifluoro-1,3-dioxobutyl)phenoxyl)-1-benzylpyrrolidine, L-SS/L-RR. X-ray crystallographic analyses reveal that the R,R configurations of the chiral carbons in the spacer induce the M helical sense of the ligand, while the S,S configurations induce the P helical sense. Through the comprehensive spectral characterization in combination with semiempirical geometry optimization using the Sparkle/RM1 model, it is confirmed that the preorganized ligands successfully control the homochirality of the helicates. Moreover, the mirror-image CD and CPL spectra and NMR measurements confirm the formation of enantiomeric pairs and their diastereopurities in solution. Detailed photophysical and chiroptical characterization studies reveal that the helicates not only exhibit intense circularly polarized luminescence (CPL) with vertical bar g(lum)vertical bar values reaching 0.10, but also show a high luminescence quantum yield of 34%. This study effectively combines the helical chirality of the helicates with the excellent sensitization ability of the beta-diketones, providing an effective strategy for the syntheses of chiral lanthanide CPL materials.
机译：β二酮是由于其优异的敏化能力而敏感镧系元素发光的最广泛使用的配体之一。然而，引入手性群体的困难将参与共轭系统的电子转变限制其在镧系元素圆偏振发光（CPL）材料中的应用。鉴于螺旋结构的固有手足性，在本文中，基于手性双β-二酮配体组装了一对同性恋四胞型束缚，Eu2L4组装，其中间隔物中的两点手性中心预组织了螺旋构象配体（3s，4s）/（3r，4r）-3,4-双（4,4'-bis（4,4,4-二氟-1,3-二氧丁基）吩氧基）-1-苄基吡咯烷，L- SS / L-RR。 X射线晶体分析揭示了垫片中的手性碳的R，R配置诱导配体的M螺旋感，而S，S配置诱导P螺旋意义。通过使用Sparkle / RM1模型结合半透态几何优化的综合光谱表征，确认预组合配体成功控制螺旋的销售。此外，镜像CD和CPL光谱和NMR测量结果证实了对映体对的形成及其在溶液中的非映射性。详细的光物理和阴压表征研究表明，螺旋不仅表现出具有垂直条G（LUM）垂直条值的强烈圆偏振的发光（CPL），达到0.10，而且显示出34％的高发发光量子产率。该研究有效地结合了螺旋液与β二酮的优异敏化能力，为手性镧系元素中的合成提供了有效的策略。

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