Electrochemically-Switched 2nd Order Non-Linear Optical Response in an Arylimido-Polyoxometalate with High Contrast and Cyclability.
Electrochemically-Switched 2nd Order Non-Linear Optical Response in an Arylimido-Polyoxometalate with High Contrast and Cyclability.
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DOI：
10.1002/anie.202215537
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发表时间：
2023-01-26
影响因子：
16.6
通讯作者：
Fielden, John
中科院分区：
文献类型：
--
作者：
Hood, Bethany R. R.;de Coene, Yovan;Torre Do Vale Froes, Afonso V. V.;Jones, Claire F. F.;Beaujean, Pierre;Liegeois, Vincent;MacMillan, Fraser;Champagne, Benoit;Clays, Koen;Fielden, John
电化学切换的二阶非线性光学响应首次在聚氧乙烯酸盐（POM）中得到证实，其中芳基酰亚胺衍生物显示出高开/关对比度（94%）、高可见光透明度和可循环性的领先组合。光谱电化学和TD-DFT研究表明，关闭是由于还原态电子跃迁的电荷转移（CT）特征减弱所致。这代表了对亚氨基-POM还原态的首次研究，并证明了POM杂化物作为电化学活化分子开关的潜力。通过还原关闭了新的芳基亚氨基聚氧乙烯酸酯（POM）中的电荷转移跃迁，从而实现了高对比度（94%）的电化学切换二阶非线性光学（NLO）响应。开/关对比度、高可见光透明度和多波长稳定性的整体组合在可切换的二阶NLO发色团中处于领先地位，并首次显示了POM杂化物作为氧化还原驱动光学开关的强大潜力。
Electrochemically switched 2nd order non‐linear optical responses have been demonstrated for the first time in polyoxometalates (POMs), with an arylimido‐derivative showing a leading combination of high on/off contrast (94 %), high visible transparency, and cyclability. Spectro‐electrochemical and TD‐DFT studies indicate that the switch‐off results from weakened charge transfer (CT) character of the electronic transitions in the reduced state. This represents the first study of an imido‐POM reduced state, and demonstrates the potential of POM hybrids as electrochemically activated molecular switches. Charge transfer transitions in a new arylimido‐polyoxometalate (POM) are turned off by reduction, enabling a high contrast (94 %) electrochemically switched 2nd order non‐linear optical (NLO) response. The overall combination of on/off contrast, high visible transparency and multicycle stability is leading in switchable 2nd order NLO chromophores, and shows for the first time the strong potential of POM hybrids as redox‐driven optical switches.
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