The development of a “two birds with one stone” strategy for capturing pollutant molecules and incorporating new functions provides a promising solution for sustainability. In this work, we designed an unprecedented deep-cavity aluminum–organic macrocycle to trap dye molecules and enhance non-linear optical performance. Using long building blocks and inorganic aluminum ions at the midriff, we successfully isolated a deep-cavity (1.8 nm) macrocycle, with a deeper cavity than classic pure organic macrocycles, such as crown ether and calixarenes. We report the accurate locking of the HAO7 dye molecule in the deep-cavity macrocycle and reveal its trapping mechanism at the molecular level for the first time. The combined host–guest compound AlOC-136-HAO7 displays altered physical properties, such as a decreased optical band gap and increased proton conductivity but also exhibits enhanced third-order non-linear optical (NLO) properties. Combined with theoretical calculations, we confirmed that the enhancement was attributed to abundant host–guest interactions and the guest-to-guest charge transfer. Our findings provide a strategy for isolating deep-cavity macrocycles and further demonstrate their enormous potential for capturing contaminants and forming valuable materials.

中文翻译：

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设计和合成深腔铝有机大环化合物以捕获染料并产生增强的非线性光学性能


开发“一石二鸟”策略来捕获污染物分子并整合新功能，为可持续发展提供了一个有前途的解决方案。在这项工作中，我们设计了一种前所未有的深腔铝有机大环化合物来捕获染料分子并增强非线性光学性能。使用长结构单元和中段的无机铝离子，我们成功分离出深腔（1.8 nm）大环化合物，其空腔比经典的纯有机大环化合物（例如冠醚和杯芳烃）更深。我们报道了HAO7染料分子在深腔大环中的精确锁定，并首次在分子水平上揭示了其捕获机制。组合的主客体化合物 AlOC-136-HAO7 显示出改变的物理特性，例如光学带隙减小和质子电导率增加，但还表现出增强的三阶非线性光学 (NLO) 特性。结合理论计算，我们证实这种增强归因于丰富的主客体相互作用和客体到客体的电荷转移。我们的研究结果提供了一种分离深腔大环化合物的策略，并进一步证明了它们在捕获污染物和形成有价值材料方面的巨大潜力。