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首页> 外文期刊>Chemistry: A European journal >Fully Fluorinated Imidodiphosphinate Shells for Visible-and NIR-Emitting Lanthanides;Hitherto Unexpected Effects of Sensitizer Fluorination on Lanthanide Emission Properties
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Fully Fluorinated Imidodiphosphinate Shells for Visible-and NIR-Emitting Lanthanides;Hitherto Unexpected Effects of Sensitizer Fluorination on Lanthanide Emission Properties

机译：全氟化亚氨基二膦酸酯壳，用于可见和近红外发射镧系元素;敏化剂氟化物迄今为止对镧系元素发射性能的意外影响

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In this paper we demonstrate that the effect of aromatic C-F substitution in ligands does not always abide by conventional wisdom for ligand design to enhance sensitisation for visible lanthanide emission,in contrast with NIR emission for which the same effect coupled with shell formation leads to unprecedented long luminescence lifetimes.We have chosen an imidodiphosphinate ligand,N-{P,P-di-(pentafluorophinoyl)}-P,P-dipentafluoro-phenylphosphinimidic acid (HF_(20)tpip),to form ideal fluorinated shells about all visible-and NIR-emitting lanthanides.The shell,formed by three ligands,comprises twelve fully fluorinated aryl sensitiser groups,yet no-high energy X-H vibrations that quench lanthanide emission.The synthesis,full characterisation including X-ray and NMR analysis as well as the photo-physical properties of the emissive complexes [Ln(F_(20)tpip)_3],in which Ln=Nd,Sm,Eu,Gd,Tb,Dy,Er,Yb,Y,Gd,are reported.The photophysical results contrast previous studies,in which fluorination of alkyl chains tends to lead to more emissive lanthanide complexes for both visible and NIR emission.Analysis of the fluorescence properties of the HF_(20)tpip and [Gd-(F(20)tpip)_3] reveals that there is a low-lying state at around 715 nm that is responsible for partially quenching of the signal of the visible emitting lanthanides and we attribute it to a pi-sigma* state.However,all visible emitting lanthanides have long lifetimes and unexpectedly the [Dy(F_(20)tpip)_3] complex shows a lifetime of 0.3 ms,indicating that the elimination of high-energy vibrations from the ligand framework is particularly favourable for Dy.The NIR emitting lanthanides show strong emission signals in powder and solution with unprecedented lifetimes.The luminescence lifetimes of [Nd(F_(20)tpip)_3],[Er(F_(20)tpip)_3] and [Yb(F_(20)tpip)_3] in deuteurated acetonitrile are 44,741 and 1111 us.The highest value observed for the [Yb(F_(20)tpip)_3] complex is more than half the value of the Yb ion radiative lifetime.
机译：在本文中，我们证明了配体中芳族CF取代的影响并不总是遵守配体设计的常规观点，以增强对可见镧系元素发射的敏感性，而NIR发射则与之相反，其相同的作用加上壳的形成导致空前的长效发光寿命。我们选择了亚氨基二亚膦酸酯配体N- {P，P-二-（五氟膦酰基）}-P，P-二五氟-苯基膦亚氨基酸（HF_（20）tpip），形成了所有可见光和周围理想的氟化壳发射NIR的镧系元素。壳由三个配体形成，包含十二个完全氟化的芳基敏化剂基团，但没有高能XH振动可抑制镧系元素的发射。合成，完整的特征包括X射线和NMR分析以及照片发光复合物[Ln（F_（20）tpip）_3]的物理性质被报道，其中Ln = Nd，Sm，Eu，Gd，Tb，Dy，Er，Yb，Y，Gd。以前的研究，其中氟化lkyl链倾向于导致可见光和NIR发射的镧系元素络合物的发射率更高。HF_（20）tpip和[Gd-（F（20）tpip）_3]的荧光性质分析表明存在一个低洼的状态在715 nm附近，负责部分消除可见发射镧系元素的信号，我们将其归因于pi-sigma *状态。但是，所有可见发射镧系元素都有很长的寿命，并且出乎意料的是[Dy（F_（20） tpip）_3]络合物的寿命为0.3 ms，表明从配体骨架中消除高能振动对Dy特别有利。NIR发射镧系元素在粉末和溶液中显示出强发射信号，具有前所未有的寿命。发光寿命氘化乙腈中[Nd（F_（20_tpip）_3]，[Er（F_（20）tpip）_3]和[Yb（F_（20_tpip）_3]的取值为44,741和1111 us。 [Yb（F_（20）tpip）_3]络合物是Yb离子辐射寿命值的一半以上。

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