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Forster Energy Transport in Metal-Organic Frameworks Is Beyond Step-by-Step Hopping

机译：金属有机框架中的Forster能量传输已超越了循序渐进的跳跃

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摘要

Metal-organic frameworks (MOFs) with light-harvesting building blocks designed to mimic photosynthetic chromophore arrays in green plants provide an excellent platform to study exciton transport in networks with well-defined structures. A step-by-step exciton random hopping model made of the elementary steps of energy transfer between only the nearest neighbors is usually used to describe the transport dynamics. Although such a nearest neighbor approximation is valid in describing the energy transfer of triplet states via the Dexter mechanism, we found it inadequate in evaluating singlet exciton migration that occurs through the Forster mechanism, which involves one-step jumping over longer distance. We measured migration rates of singlet excitons on two MOFs constructed from truxene-derived ligands and zinc nodes, by monitoring energy transfer from the MOF skeleton to a coumarin probe in the MOF cavity. The diffusivities of the excitons on the frameworks were determined to be 1.8 × 10~(-2) cm~2/s and 2.3 × 10~(-2) cm~2/s, corresponding to migration distances of 43 and 48 nm within their lifetimes, respectively. "Through space" energy-jumping beyond nearest neighbor accounts for up to 67% of the energy transfer rates. This finding presents a new perspective in the design and understanding of highly efficient energy transport networks for singlet excited states.
机译：带有光收集构件的金属有机框架（MOF）旨在模拟绿色植物中的光合作用生色团阵列，为研究结构明确的网络中的激子传输提供了一个极好的平台。通常使用由仅最近邻之间的能量传输的基本步骤构成的逐步激子随机跳跃模型来描述传输动力学。尽管这样的最近邻近似在描述通过德克斯特机制进行的三重态的能量转移时是有效的，但我们发现它不足以评估通过福斯特机制发生的单重态激子迁移，这涉及一步跃越长距离。我们通过监测从MOF骨架到MOF腔体中香豆素探针的能量转移，测量了从茂铁衍生的配体和锌节点构建的两个MOF上单重态激子的迁移速率。确定激子在骨架上的扩散度为1.8×10〜（-2）cm〜2 / s和2.3×10〜（-2）cm〜2 / s，对应于43 nm和48 nm的迁移距离他们的一生。 “越过空间”能量跃迁到最近的邻居占能量传输率的67％。这一发现为单重激发态的高效能量传输网络的设计和理解提供了新的视角。

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  • 来源
    《Journal of the American Chemical Society》 |2016年第16期|5308-5315|共8页
  • 作者

    Qiongqiong Zhang; Cankun Zhang; Lingyun Cao; Zi Wang; Bing An; Zekai Lin; Ruiyun Huang; Zhiming Zhang; Cheng Wang; Wenbin Lin;

  • 作者单位

    Collaborative Innovation Center of Chemistry for Energy Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, PR China;

    Collaborative Innovation Center of Chemistry for Energy Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, PR China;

    Collaborative Innovation Center of Chemistry for Energy Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, PR China;

    Collaborative Innovation Center of Chemistry for Energy Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, PR China;

    Collaborative Innovation Center of Chemistry for Energy Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, PR China;

    Department of Chemistry, University of Chicago, 929 E 57th Street, Chicago, Illinois 60637, United States;

    Collaborative Innovation Center of Chemistry for Energy Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, PR China;

    Collaborative Innovation Center of Chemistry for Energy Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, PR China,Key Laboratory of Polyoxometalate Science of the Ministry of Education, Faculty of Chemistry, Northeast Normal University, Changchun, Jilin 130024, PR China;

    Collaborative Innovation Center of Chemistry for Energy Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, PR China;

    Collaborative Innovation Center of Chemistry for Energy Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, PR China,Department of Chemistry, University of Chicago, 929 E 57th Street, Chicago, Illinois 60637, United States;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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  • 正文语种 eng
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  • 入库时间 2022-08-18 03:08:45

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